O2 activation and 1O2 generation over phosphate modified BiOCl for efficient photodegradation of organic pollutants
作者：
Xu, Hua;Liu, Xiangming;Li, Hao;Zhang, Lizhi
期刊：
Applied Catalysis B: Environmental ,2022年314:121520 ISSN：0926-3373
通讯作者：
Xu, H;Li, H
作者机构：
[Xu, Hua; Liu, Xiangming; Xu, H] Wuhan Inst Technol, Sch Chem & Environm Engn, Wuhan 430205, Peoples R China.;[Zhang, Lizhi; Li, H; Li, Hao] Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Li, H ] C;[Xu, H ] W;Wuhan Inst Technol, Sch Chem & Environm Engn, Wuhan 430205, Peoples R China.;Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
1O2 generation;BiOCl;O2 activation;Phosphate modification;Photocatalysis
摘要：
Phosphate modification over semiconductor photocatalyst was an effective route to promote photodegradation of organic pollutants. Studies on promoted O2 adsorption, better charge separation, and free ∙OH radicals raised from phosphate modification are clear, whereas O2 activation and the generated reactive oxygen species (·O2-, H2O2, and 1O2) have been ignored. Herein, the hydrogen bond network constructed between BiOCl surface and phosphate weaken the surface Bi-O bond thus benefit the formation of oxygen vacancy (OVs). OVs not only facilitate the adsorption of organic pollutants but also promote the O2 activation to generate H2O2 and 1O2. Another route for 1O2 generation relies on the H2O2 reacted with HClO from lattice chlorine oxidation was demonstrated. The directly attack of surface adsorbed 4-CP via h+, in addition with the selective oxidation via 1O2, synergetically contribute excellent photodegradation performance. This study systematically reveals the O2 activation and 1O2 generation for efficient photodegradation over phosphate modified BiOCl. © 2022 Elsevier B.V.
语种：
英文
展开
Local Spatial Polarization Induced Efficient Charge Separation of Squaraine-Linked COF for Enhanced Photocatalytic Performance
作者：
Ben, Haijie;Yan, Gaojie;Liu, Haiyang;Ling, Cancan;Fan, You* ;...
期刊：
Advanced Functional Materials ,2022年32(14):2104519- ISSN：1616-301X
通讯作者：
Zhang, Xiaojie;Fan, You
作者机构：
[Yan, Gaojie; Ben, Haijie; Zhang, Xiaojie; Liu, Haiyang] Hebei Univ Technol, Dept Polymer Mat & Engn, Hebei Key Lab Funct Polymers, 8 Guangrong St, Tianjin 300130, Peoples R China.;[Ling, Cancan; Ben, Haijie; Fan, You] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构：
[Zhang, Xiaojie] H;[Fan, You] C;Hebei Univ Technol, Dept Polymer Mat & Engn, Hebei Key Lab Funct Polymers, 8 Guangrong St, Tianjin 300130, Peoples R China.;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词：
charge separation;covalent organic frameworks;local charge polarization;photocatalysts;zwitterionic resonance structures
摘要：
The efficiencies of semiconductor photocatalysis are always severely restricted by the rapid recombination of charge carriers in the bulk phase, while local polarization is an efficient scenario to conquer the above issue to boost the photocatalytic performance. Here, as a proof-of-concept demonstration, local charge polarization induced by the intrinsic zwitterionic resonance structure of photocatalysts is reported. A novel squaraine-based covalent organic framework (SQ-COF-1) photocatalyst with an interesting zwitterionic resonance structure is creatively developed. Meanwhile, the comparison samples (SQ-COF-2 and PDA-COF) based on similar COF structure with tunable local polarity are accordingly designed and prepared. The local charge polarization generated from the zwitterionic resonance structure profoundly redistributes and separates the charge carriers, as evidenced by experimental and theoretical results collectively. Benefiting by the largest local polarization, SQ-COF-1 exhibits superior visible-light-driven photocatalytic activities than SQ-COF-2, PDA-COF, and commonly used polymeric carbon nitride photocatalyst. This work presents a local charge polarization protocol for engineering charge behavior to promote photocatalysis, which shows great promise for the future design of high-performance photocatalytic materials. © 2021 Wiley-VCH GmbH.
语种：
英文
展开
Temperature-Responsive Nanocarrier-Regulated Alternative Release of ?Cargos? for a Multiplex Photoelectrochemical Bioassay of Antibiotic-Resistant Genes
作者：
Liu, Lijuan;Li, Xin;Yao, Qingfeng;Hu, Yachen;Sun, Hongwei;...
期刊：
Analytical Chemistry ,2022年94(40):14061-14070 ISSN：0003-2700
通讯作者：
Gong, Jingming(jmgong@mail.ccnu.edu.cn)
作者机构：
[Liu, Lijuan; Zhang, Lizhi; Gong, Jingming; Yao, Qingfeng; Sun, Hongwei; Hu, Yachen; Li, Xin] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Jingming Gong] K;Key Laboratory of Pesticide and Chemical Biology of the Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
摘要：
A smart temperature stimuli-driven multiplex photoelectrochemical (PEC) assay was constructed for antibiotic resistance genes (ARGs) detection, where the stimuli-responsive gatekeeping by regulating the alternative release of "cargo" allowed for the simultaneous detection of multiple tetracycline resistance gene, using tetA (T(DNA1)) and tetC (T(DNA2)) as the model. Dual temperature-responsive nanoassemblies were embedded in the PEC bioassay as signal DNA tages: one thermoresponsive polymer (poly(N-isopropylacrylamide), PNIPAM)-capped mesoporous silica nanoparticles (MSN) with loading the "cargo" of HgO nanoparticles as signal DNA1 tags (S(DNA1)-PNIPAM@MSN@HgONPs) and the other antimony tartrate (SbT)-anchored silica nanospheres as signal DNA2 tags (S(DNA2)-SbT@SiO(2)NSs). At 20 °C, below the lower critical solution temperature (LCST) of PNIPAM, the "gatekeeper" PNIPAM in S(DNA1)-PNIPAM@MSN@HgONPs was in an ON state, igniting Hg(2+) release through the pore of SiO(2). While at above LCST (40 °C), it was in an OFF state. Likewise, the thermo-dependent dissociation of SbT endowed the grafted S(DNA2) tags switching from the OFF (at 20 °C) to ON state (at 40 °C), igniting SbO(+) release. The released Hg(2+) and SbO(+) triggered the amplified photocurrents due to the structure evolution of the photoactive layer into HgS/ZnS or Sb(2)S(3)/ZnS heterostructure, thus achieving sensitive detection of multiple ARGs: tetA, tetC, tetG, tetM, tetO, tetZ, tetX, and tetW. Combined with heat map analysis, rapid screening of the ARGs profiles in 12 samples could be realized. This bioassay is simple and accessible for multiple genes analysis with the detection limit down to 0.50 nM. And it was successfully applied for measuring tetracycline ARGs in real sludge samples.
语种：
英文
展开
A Pd2+-Free Near-Infrared Fluorescent Probe Based on Allyl Ether Isomerization for Tracking CORM-3 with High Contrast Imaging in Living Systems
作者：
Gong, Shengyi;Zhou, Enbo;Liu, Yijia;Gui, Zhisheng;Feng, Guoqiang*
期刊：
Analytical Chemistry ,2022年94(4):2042-2047 ISSN：0003-2700
通讯作者：
Feng, Guoqiang
作者机构：
[Feng, Guoqiang; Gong, Shengyi; Feng, GQ; Liu, Yijia; Gui, Zhisheng; Zhou, Enbo] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Feng, GQ ] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要：
As a CO donor, CORM-3 is widely used nowadays to study the role of CO as a gasotransmitter and potential drug in biological systems. Developing methods to detect CORM-3 in live systems will contribute to these studies. Herein, we developed a novel Pd2+-free near-infrared fluorescent probe CORM3-AE for detecting CORM-3 both in live cells and in vivo. We found that the allyl ether group in CORM3-AE could be cleaved by CORM-3 directly via an isomerization process to release the NIR fluorophore QCy7 and cause distinct NIR fluorescence changes. Importantly, CORM3-AE responds quickly and shows high sensitivity and selectivity for CORM-3 with NIR fluorescence turn-on changes at 743 nm (λex = 662 nm), and when the excitation wavelength is 450 nm, CORM3-AE can respond to CORM-3 with ratiometric fluorescence signals at 743/605 nm. Moreover, CORM3-AE can track CORM-3 in live cells and animals with excellent imaging performance. Thus, this work not only provides a powerful new tool for CORM-3 detection in live systems but also provides a new method to construct CORM-3 probes by allyl ether isomerization. © 2022 American Chemical Society
语种：
英文
展开
Rare earth La single atoms supported MoO3-x for efficient photocatalytic nitrogen fixation
作者：
Liu, Xiufan;Luo, Yani;Ling, Cancan;Shi, Yanbiao;Zhan, Guangming;...
期刊：
Applied Catalysis B: Environmental ,2022年301:120766 ISSN：0926-3373
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Gu, Huayu; Wei, Kai; Ling, Cancan; Zhang, Lizhi; Liu, Xiufan; Guo, Furong; Li, Hao; Zhan, Guangming; Zhang, LZ; Ai, Zhihui; Luo, Yani] Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Shi, Yanbiao] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Coordination;MoO3−x;Photocatalytic nitrogen fixation;Rare-earth La;Single-atom catalyst
摘要：
Herein, we demonstrate that the rare-earth La single catalyst with multi-shell characteristic is an excellent choice for this purpose. By merit of its unsaturated orbitals of La, the single La atom strongly bonds with the two-coordinated lattice oxygen on the oxygen-deficient MoO3−x to form O2c-La-O2c coordination. This robust metal-support interaction frees single atoms from detachment or aggregation, and prevents catalyst from deactivation. Meanwhile, the occupied 5d orbitals of La back-donate electrons to the 2π* molecular orbitals of adsorbed N2 that substantially activate the inert N[tbnd]N bond towards successive hydrogenation. And single La atom could optimize the electron property of the MoO3−x support to promote photocatalytic nitrogen fixation. Without any sacrificial agents, this single atom La catalyst with a well-designed coordination structure delivers an impressive NH3 production rate of 209.0 μmol h[sbnd]1 g [sbnd]1 under visible light, outperforming most reported single atom photocatalysts. © 2021 Elsevier B.V.
语种：
英文
展开
Chiral Covalent Organic Framework Packed Nanochannel Membrane for Enantioseparation
作者：
Dr. Siyun Zhang;Prof. Juan Zhou;Prof. Haibing Li
期刊：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2022年61(27):e202204012- ISSN：1433-7851
通讯作者：
Li, Haibing(lhbing@mail.ccnu.edu.cn);Zhou, Juan(zhoujuan@wh.iov.cn)
作者机构：
[Zhang, Siyun; Li, Haibing] Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan;430079, China;College of Chemical Engineering, North China University of Science and Technology, Tangshan;063210, China;[Zhou, Juan] State Key Laboratory of Virology, Wuhan Institute of Virology, Center for Biosafety Mega-Science, Chinese Academy of Sciences, Wuhan
通讯机构：
[Prof. Juan Zhou] S;[Prof. Haibing Li] K;Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China<&wdkj&>State Key Laboratory of Virology, Wuhan Institute of Virology, Center for Biosafety Mega-Science, Chinese Academy of Sciences, Wuhan, 430071 P. R. China
关键词：
Chiral Drugs;Covalent Organic Frameworks;Enantioseparation;Nanochannels
摘要：
A nanochannel membrane has the prospect of large-scale separation. However, selectivity in enantioseparation is a challenge, due to the size difference between nanochannels and enantiomers. Here, we compartmented nanochannels by the in situ synthesis of a L-tyrosine functionalized covalent organic framework (L-Tyr-COF). The L-Tyr-COF decreased the pore size of channels to match with naproxen enantiomers (S/R-NPX) and improved the enantioselective gating. In contrast to the surface-functionalized nanochannels (L-Tyr channel), the L-Tyr-COF packed nanochannels (L-Tyr-COF channel) exhibited high enantioselectivity for S-NPX and realized the enantioseparation with the enantiomer excess value up to 94.2 %. The separation flux through the highly porous L-Tyr-COF channel was 1.33 mmol m−2 h−1. This study provided a size-matching strategy and the chiral covalent organic framework packed nanochannel membrane to realize enantioseparation with high selectivity and flux. © 2022 Wiley-VCH GmbH.
语种：
英文
展开
Highly Improved Chiral-Selective Resolution in Pillar[5]arene-Functionalized Molecularly Imprinted Membranes
作者：
Wang, Li;Li, Guang;Yang, Lei;Qu, Haonan;Cheng, Jing;...
期刊：
ACS APPLIED POLYMER MATERIALS ,2022年4(9):6723-6730 ISSN：2637-6105
通讯作者：
Cheng, Jing(chengjingok@mail.ccnu.edu.cn);Li, Haibing(lhbing@mail.ccnu.edu.cn)
作者机构：
[Wang, Li; Li, Guang; Yang, Lei; Li, Haibing; Cheng, Jing; Qu, Haonan] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Barakat, Dalia A.; Abdallah, Mohammed] Cairo Univ, Fac Agr, Dept Econ Entomol & Pesticides, Giza 12411, Egypt.
通讯机构：
[Jing Cheng; Haibing Li] K;Key Laboratory of Pesticide and Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, P. R China
关键词：
chiral separation;membrane separation;molecularly imprinted polymer;pillar[5]arenes;S/R-triadimefon
摘要：
It is a challenging task to achieve the effective separation of chiral compounds under simple and rapid conditions. In order to solve this problem, this study used the molecularly imprinted membrane (MIM) technology developed on the basis of biological semi-permeable membranes, using S-triadimefon as the template molecule, and successfully prepared MIMs by photo-initiated polymerization. By adding macrocyclic molecular 1,4-bis(allyloxy)pillar[5]arene as a functional monomers, the effectiveness of the chiral recognition sites of the target molecules is improved, thereby improving the chiral selectivity of the MIM and optimizing the molar ratio of template molecules, monomers, and cross-linkers. On this basis, the separation effect of non-MIM (NIM), single-monomer MIM (MIM-I), and two-monomer MIM (MIM-II) on triadimefon enantiomers was investigated. It was found that the enantiomer excess (e. e.) % value of MIM-I is larger than that of NIM, but the value of MIM-I is still very low. When pillar[5]arene, a macrocyclic molecule was added as the second monomer, its e. e. % increased from 27.4 to 84.8%. © 2022 American Chemical Society.
语种：
英文
展开
Molecular Design and Photothermal Application of Thienoisoindigo Dyes with Aggregation-Induced Emission
作者：
Chen, Weijie;Chen, Huijuan;Huang, Yurou;Tan, Ying;Tan, Chunyan;...
期刊：
ACS Applied Bio Materials ,2022年5(7):3428-3437 ISSN：2576-6422
通讯作者：
Yin, Jun(yinj@mail.ccnu.edu.cn);Tan, Ying(tan.ying@sz.tsinghua.edu.cn);Tan, Chunyan(tancy@sz.tsinghua.edu.cn)
作者机构：
[Chen, Weijie; Chen, Huijuan; Huang, Yurou; Yin, Jun] Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan;430079, China;[Tan, Ying; Tan, Chunyan] State Key Laboratory of Chemical Oncogenomics, Key Laboratory of Chemical Biology, Shenzhen International Graduate School, Tsinghua University, Guangdong, Shenzhen;518055, China;[Xie, Yuan] Guangdong Provincial Key Laboratory of Radioactive and Rare Resource Utilization, Shaoguan
通讯机构：
[Ying Tan; Chunyan Tan] S;[Jun Yin] K;Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China<&wdkj&>State Key Laboratory of Chemical Oncogenomics, Key Laboratory of Chemical Biology, Shenzhen International Graduate School, Tsinghua University, Shenzhen, Guangdong 518055, P. R. China
关键词：
aggregation-induced emission (AIE);fluorescent dyes;photothermal therapy (PTT);tetraphenylethene;thienoisoindigo
摘要：
Organic fluorescent dyes with aggregation-induced emission (AIE) property have an extensive application range, especially in the fields of imaging, labeling, and adjusting microprocesses in aggregated environments. In particular, the thienoisoindigo skeleton, which exhibits an outstanding electron-withdrawing capacity in optoelectronic materials, has been defined as a promising AIE candidate. For instance, by installing AIE blocks or other rotatable groups at two terminal sites, such as various arylamine groups, thienoisoindigo derivatives can be efficiently turned to be functional AIE structures. In this work, a thienoisoindigo derivative with AIE characteristics, namely, TII-TPE, was developed. This AIE system was expanded by linking typical AIE fragments, namely, tetraphenylethene, with the proposed thienoisoindigo derivative, which exhibited typical AIE fluorescence in the 600-850 nm range and maintained high photostability. Then, employing the reported derivative TII-TPA coating thienoisoindigo and triphenylamine as a contrast, aggregated TII-TPE and TII-TPA nanoparticles were prepared and demonstrated photothermal conversion efficiencies of 36.2 and 35.6%, respectively. Moreover, both nanoparticles were evaluated as photothermal therapeutic (PTT) agents in a tumor mouse model, which showed to significantly inhibit tumor growth after four treatment cycles in vivo. This work not only presents an enriched thienoisoindigo system but also provides a pattern for subsequent construction of functional AIE molecules. © 2022 American Chemical Society. All rights reserved.
语种：
英文
展开
An Electrochemical Strategy for Simultaneous Heavy Metal Complexes Wastewater Treatment and Resource Recovery
作者：
Li, Meiqi;Chen, Na;Shang, Huan;Ling, Cancan;Wei, Kai;...
期刊：
Environmental Science & Technology ,2022年56(15):10945-10953 ISSN：0013-936X
通讯作者：
Ai, Zhihui(jennifer.ai@mail.ccnu.edu.cn);Zhang, Lizhi(zhanglz@mail.ccnu.edu.cn)
作者机构：
[Wei, Kai; Ling, Cancan; Zhang, Lizhi; Shang, Huan; Chen, Na; Zhao, Shengxi; Jia, Falong; Ai, Zhihui; Li, Meiqi; Zhou, Biao] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Zhang, Lizhi] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China.
通讯机构：
[Zhihui Ai; Lizhi Zhang] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China<&wdkj&>School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
关键词：
Cu recovery;decomplexation;electro-Fenton;heavy metal−organic complexes;sodium tetrapolyphosphate electrolyte
摘要：
Heavy metals chelated with coexisting organic ligands in wastewater impose severe risks to public health and the ambient ecosystem but are also valuable metal resources. For sustainable development goals, the treatment of heavy metal complexes wastewater requires simultaneous metal-organic bond destruction and metal resource recovery. In this study, we demonstrated that a neutral pH electro-Fenton (EF) system, which was composed of an iron anode, carbon cloth cathode, and sodium tetrapolyphosphate electrolyte (Na6TPP), could induce a successive single-electron activation pathway of molecular oxygen due to the formation of Fe(II)-TPP complexes. The boosted •OH generation in the Na6TPP-EF process could decomplex 99.9% of copper ethylene diamine tetraacetate within 8 h; meanwhile, the released Cu ions were in situ deposited on the carbon cloth cathode in the form of Cu nanoparticles with a high energy efficiency of 2.45 g kWh-1. Impressively, the recovered Cu nanoparticles were of purity over 95.0%. More importantly, this neutral EF strategy could realize the simultaneous removal of Cu, Ni, and Cr complexes from real electroplating effluents. This study provides a promising neutral EF system for simultaneous heavy metal complexes wastewater treatment and resource recovery and sheds light on the importance of molecular oxygen activation in the field of pollutant control. © 2022 American Chemical Society. All rights reserved.
语种：
英文
展开
Oxygen Vacancy-Governed Opposite Catalytic Performance for C3H6 and C3H8 Combustion: The Effect of the Pt Electronic Structure and Chemisorbed Oxygen Species
作者：
Fang, Yarong;Li, Huijuan;Zhang, Qi;Wang, Chenyang;Xu, Jue;...
期刊：
Environmental Science & Technology ,2022年56(5):3245-3257 ISSN：0013-936X
通讯作者：
Luo, Zhu;Guo, Yanbing
作者机构：
[Zhang, Qi; Wang, Chenyang; Guo, Yanbing; Li, Huijuan; Xu, Jue; Yang, Ji; Zhu, Yuhua; Guo, YB; Luo, Zhu; Shen, Huan; Pan, Chuanqi; Fang, Yarong] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Guo, YB ; Luo, Z] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
oxygen vacancy;Pt catalysts;chemisorbed peroxide oxygen;C3H6 and C3H8 oxidation
摘要：
Revealing the role of engineered surface oxygen vacancies in the catalytic degradation of volatile organic compounds (VOCs) is of importance for the development of highly efficient catalysts. However, because of various structures of VOC molecules, the role of surface oxygen vacancies in different catalytic reactions remains ambiguous. Herein, a defective Pt/TiO2-x catalyst is proposed to uncover the different catalytic mechanisms of C3H6 and C3H8 combustion via experiments and theoretical calculations. The electron transfer, originated from the oxygen vacancy, facilitates the formation of reduced Pt0 species and simultaneously interfacial chemisorbed O2, thus promoting the C3H6 combustion via efficient C═C cleavage. The reduced Pt nanoparticles facilitate the robust chemisorption of bridging dimer O22- (Pt-O-O-Ti) species. This chemisorbed oxygen inhibits the C3H8 combustion by depressing C3H8 adsorption. This work offers insights for the rational design of highly efficient catalysts for activating the C═C bond in alkene or C-H bond in alkane. © 2022 American Chemical Society
语种：
英文
展开
Vacancy-Rich and Porous NiFe-Layered Double Hydroxide Ultrathin Nanosheets for Efficient Photocatalytic NO Oxidation and Storage
作者：
Li, Hao;Zhu, Huijun;Shi, Yanbiao;Shang, Huan;Zhang, Lizhi;...
期刊：
Environmental Science & Technology ,2022年56(3):1771-1779 ISSN：0013-936X
通讯作者：
Wang, Jing
作者机构：
[Li, Hao; Wang, Jing] Inst Environm Engn, CH-8093 Zurich, Switzerland.;[Li, Hao; Wang, Jing] Empa, Swiss Fed Labs Mat Sci & Technol, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.;[Zhu, Huijun] Linkoping Univ, S-58183 Linkoping, Sweden.;[Zhang, Lizhi; Shi, Yanbiao] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China.;[Zhang, Lizhi; Shang, Huan] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Wang, Jing] I;[Wang, Jing] S;Inst Environm Engn, CH-8093 Zurich, Switzerland.;Swiss Fed Labs Mat Sci & Technol, Empa, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.
关键词：
photocatalysis;NO removal;layered double hydroxide;environmental control;nitrate storage
摘要：
An appealing strategy in the direction of circular chemistry and sustainable nitrogen exploitation is to efficiently convert NOx pollutants into low-toxic products and simultaneously provide crop plants with metabolic nitrogen. This study demonstrates that such a scenario can be realized by a defect- and morphology-coengineered Ni-Fe-layered double hydroxide (NiFe-LDH) comprising ultrathin nanosheets. Rich oxygen vacancies are introduced onto the NiFe-LDH surface, which facilitate charge carrier transfer and enable photocatalytic O2 activation into superoxide radicals (•O2-) under visible light. •O2- on NiFe-LDH thermodynamically oxidizes NO into nitrate with selectivity over 92%, thus suppressing dangerous NO2 emissions. By merit of abundant mesopores on NiFe-LDH ultrathin nanosheets bearing a high surface area (103.08 m2/g), nitrate can be readily stored without compromising the NO oxidation reactivity or selectivity for long-term usage. The nitrate species can be easily washed off the NiFe-LDH surface and then enriched in the liquid form as easy-to-use chemicals. © 2022 American Chemical Society.
语种：
英文
展开
A protein vaccine with Alum/c-GAMP/poly(I:C) rapidly boosts robust immunity against SARS-CoV-2 and variants of concern
作者：
Zhang, Ru-Yan;Yin, Xu-Guang;Zhou, Shi-Hao;Zhang, Hai-Wei;Lu, Jie;...
期刊：
Chemical Communications ,2022年58(24):3925-3928 ISSN：1359-7345
通讯作者：
Yang, Guang-Fu;Guo, J;Gong, R
作者机构：
[Wang, Jian; Liu, Yan-Ling; Feng, Ran-Ran; Wen, Yu; Yin, Xu-Guang; He, Chen-Bin; Zhou, Shi-Hao; Li, Yu-Ting; Yang, Guang-Fu; Zhang, Ru-Yan; Lu, Jie; Ding, Dong; Guo, J; Guo, Jun] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ,Hubei I, Wuhan 430079, Peoples R China.;[Gong, Rui; Zhang, Hai-Wei; Gong, R] Chinese Acad Sci, Ctr Biosafety Megasci, Wuhan Inst Virol, CAS Key Lab Special Pathogens & Biosafety, Wuhan 430071, Peoples R China.;[Wei, Hua-Wei] Jiangsu East Mab Biomed Technol Co Ltd, Nantong 226499, Peoples R China.
通讯机构：
[Guo, J ; Yang, GF; Gong, R ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ,Hubei I, Wuhan 430079, Peoples R China.;Chinese Acad Sci, Ctr Biosafety Megasci, Wuhan Inst Virol, CAS Key Lab Special Pathogens & Biosafety, Wuhan 430071, Peoples R China.
摘要：
Adjuvants are important components in vaccines to increase the immunogenicity of proteins and induce optimal immunity. In this study, we designed a novel ternary adjuvant system Alum + c-GAMP + poly(I:C) with STING agonist 3,3′-c-GAMP (c-GAMP) and TLR3 agonist poly(I:C) co-adsorbed on the conventional adjuvant aluminum gel (Alum), and further constructed an S1 protein vaccine. Two doses of vaccination with the ternary adjuvant vaccine were sufficient to induce a balanced Th1/Th2 immune response and robust humoral and cellular immunity. Additionally, the ternary adjuvant group had effective neutralizing activity against live virus SARS-CoV-2 and pseudovirus of all variants of concern (alpha, beta, gamma, delta and omicron). These results indicate that the ternary adjuvants have a significant synergistic effect and can rapidly trigger potent immune responses; the combination of the ternary adjuvant system with S1 protein is a promising COVID-19 vaccine candidate. © 2022 The Royal Society of Chemistry
语种：
英文
展开
Intrinsically-ionic donor-acceptor molecules featuring thermally-activated delayed fluorescence for high-performance host-guest blue light-emitting electrochemical cells
作者：
Pang, Xianchun;Zhang, Ke;Song, Yongjun;Xiu, Yue;Yu, Renyou;...
期刊：
Chemical Engineering Journal ,2022年450:137987 ISSN：1385-8947
通讯作者：
He, Lei(helei@ccnu.edu.cn)
作者机构：
[Zhang, Ke; Song, Yongjun; Pang, Xianchun; Xiu, Yue; He, Lei; Yu, Renyou] Cent China Normal Univ, Coll Chem, Key Lab Pesticide, Chem Biol Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Lei He] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
关键词：
Blue;Donor–acceptor molecule;Host–guest;Ionic;Light-emitting electrochemical cell;Thermally activated delayed fluorescence
摘要：
High-performance blue light-emitting electrochemical cells (LECs) have remained a formidable challenge. Ionic donor–acceptor molecules, especially those featuring thermally-activated delayed fluorescence (TADF), are promising hosts for developing high-performance blue LECs, but such hosts have remained undeveloped. Here, we report two intrinsically-ionic donor–acceptor molecules, 1-(3-(4-(4-(3,6-di-tert-butyl-9H-carbazol-9-yl)phenyl)-6-phenylpyrimidin-2-yl)phenyl)-3-ethyl-1H-imidazol-3-ium hexafluorophosphate (H1) and 1-(3-(4-(2-(3,6-di-tert-butyl-9H-carbazol-9-yl)phenyl)-6-phenylpyrimidin-2-yl)phenyl)-3-ethyl-1H-imidazol-3-ium hexafluorophosphate (H2), and their use as hosts for high-performance blue LECs. 3,6-di-tert-butylcabazole and imidazolium-substituted 2,4-diphenylpyrimidine are used as the donor and acceptor, respectively, which are located para (for H1) or ortho (for H2) to each other on the central phenyl linker. While H1 shows a low triplet energy (<2.6 eV), a large singlet–triplet energy gap (ΔEST) (>0.4 eV) and no TADF, H2 exhibits a high triplet energy (>2.8 eV), a small ΔEST (∼0.2 eV) and distinct TADF, due to its twisted donor–acceptor conformation. Both H1 and H2 show excellent electrochemical stability. Host-guest blue LECs using H2 as the host and a phosphorescent cationic Ir(III) complex as the guest afford sky-blue electroluminescence with high blue-color stability and peak brightness/peak external quantum efficiency/half-lifetime at 1078 cd m−2/8.6%/66 min under a constant-current driving. Upon adding LiPF6 into the active layer, a half-lifetime of ∼ 2 h is achieved at 918 cd m−2. These performances are the highest for host–guest blue LECs reported so far. The efficiencies and operational stability achieved at the high brightness are also the highest for blue LECs with inert-metal cathodes reported so far. © 2022 Elsevier B.V.
语种：
英文
展开
Fast detection of isocarbophos using bis-propargylcalix[4]arene-stabilized silver nanoparticles
作者：
Hu, Hao;Liu, Zhuo;Li, Guang;Hu, Heng;Qu, Yanjuan;...
期刊：
Analytical Sciences ,2022年38(6):861-867 ISSN：0910-6340
通讯作者：
Qu, Yanjuan(quyanjuan@znhospital.cn);Lu, Minxiang(luminxiang@znhospital.cn);Liang, Feng(feng_liang@wust.edu.cn);Li, Haibing(lhbing@mail.ccnu.edu.cn)
作者机构：
[Qu, Yanjuan; Hu, Hao] Wuhan Univ, Zhongnan Hosp, Dept Radiol, 169 East Lake Rd, Wuhan 430071, Hubei, Peoples R China.;[Hu, Heng] Huazhong Univ Sci & Technol, Tongji Med Coll, Liyuan Hosp, Dept Resp & Crit Care Med, East Lake Rd, Wuhan 430071, Hubei, Peoples R China.;[Lu, Zhiyan; Liu, Zhuo; Lu, Minxiang] Wuhan Univ, Zhongnan Hosp, Dept Forens Med, 169 East Lake Rd, Wuhan 430071, Hubei, Peoples R China.;[Liang, Feng] Wuhan Univ Sci & Technol, Sch Chem & Chem Engn, Wuhan 430065, Hubei, Peoples R China.;[Li, Guang; Li, Haibing] Cent China Normal Univ, Minist Educ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Yanjuan Qu; Minxiang Lu] D;[Feng Liang] S;[Haibing Li] K;Department of Radiology, Zhongnan Hospital of Wuhan University, Wuhan, People’s Republic of China<&wdkj&>Department of Forensic Medicine, Zhongnan Hospital of Wuhan University, Wuhan, People’s Republic of China<&wdkj&>School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, People’s Republic of China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, People’s Republic of China
关键词：
Bis-propargylcalix[4]arene;Silver nanoparticles;Isocarbophos;Colorimetric
摘要：
Bis-propargylcalix[4]arene-stabilized silver nanoparticles (BPCA–Ag NPs), as a chemosensor for detecting an isocarbophos (ICP) pesticide in an aqueous medium, are reported in this work. The nanoparticles were characterized by UV–visible spectroscopy, dynamic light scattering, zeta potential and high-resolution transmission electron microscopy techniques. It was observed that the BPCA–Ag NPs had a high selectivity for isocarbophos with a detection limit of 1.0 × 10–6M. According to the result of this research, the BPCA–Ag NPs were found to be useful for the colorimetric detection of isocarbophos in an aqueous medium. It provides a new method for in situ detection of isocarbophos using host–guest interaction. Graphical abstract: [Figure not available: see fulltext.] © 2022, The Author(s), under exclusive licence to The Japan Society for Analytical Chemistry.
语种：
英文
展开
Nitrogen-Doped Carbon as a Highly Active Metal-Free Catalyst for the Selective Oxidative Dehydrogenation of N-Heterocycles
作者：
Li, Xun;Yuan, Ziliang;Liu, Yi;Yang, Hanmin;Nie, Jiabao;...
期刊：
ChemSusChem ,2022年15(15):e202200753- ISSN：1864-5631
通讯作者：
Yang, Hanmin(yanghanmin@sina.com);Liu, Bing(liubing@mail.scuec.edu.cn)
作者机构：
[Liu, Bing; Li, Xun; Yang, Hanmin; Nie, Jiabao; Yuan, Ziliang] South Cent Minzu Univ, Key Lab Catalysis & Energy Mat Chem, Minist Educ, Wuhan 430074, Peoples R China.;[Wang, Guanghui; Yuan, Ziliang] Wuhan Univ Sci & Technol, Coll Chem Engn & Technol, Hubei Coal Convers & New Carbon Mat Key Lab, Wuhan 430081, Peoples R China.;[Liu, Yi] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Prof. Hanmin Yang; Prof. Bing Liu; Prof. Hanmin Yang Prof. Hanmin Yang Prof. Hanmin Yang; Prof. Bing Liu Prof. Bing Liu Prof. Bing Liu] K;Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education, South-Central Minzu University, Wuhan, 430074 P. R. China
关键词：
metal-free;N-heteroarenes;N-heterocyclic compounds;nitrogen-doped carbon materials;oxidative dehydrogenation
摘要：
N-heteroarenes represents one of the most important chemicals in pharmaceuticals and other bio-active molecules, which can be easily accessed from the oxidation of N-heterocycles over metal catalysts. Herein, the metal-free oxidative dehydrogenation of N-heterocycles into N-heteroarenes was developed using molecular oxygen as the terminal oxidant. The nitrogen-doped carbon materials were facilely prepared via the simple pyrolysis process using biomass (carboxymethyl cellulose sodium) and dicyandiamide as the carbon and nitrogen source, respectively, and they were discovered to be robust for the oxidative dehydrogenation of N-heterocycles into N-heteroarenes under mild conditions (80 °C under 1 bar O2) with water as the green solvent. Diverse N-heterocycles including 1,2,3,4-tetrahydroisoquinolines, indolines and 1,2,3,4-tetrahydroquinoxalines were smoothly converted into N-heteroarenes with high to excellent yields (76–>99 %). Superoxide radical (⋅O2−) and hydroxyl radical (⋅OH) were probed as the reactive oxygen species for the oxidation of N-heterocycles into N-heteroarenes. More importantly, the nitrogen-doped carbon catalyst can be reused with a high stability. The method provides an environmentally friendly and economical route to access important N-hetero-aromatic commodities. © 2022 Wiley-VCH GmbH.
语种：
英文
展开
Study on the environmental fate of three insecticides in garlic by in vivo sampling rate calibrated-solid phase microextraction-gas chromatography-mass spectrometry
作者：
Chen, Tiantian;Yu, Xinhe;Tian, Xinmeng;Hu, Jiajia;Chen, Yanyan;...
期刊：
Food Chemistry ,2022年367:130740 ISSN：0308-8146
通讯作者：
Xu, Hui;Yang, Guang-Fu
作者机构：
[Yu, Xinhe; Long, Guangdou; Yang, Guang-Fu; Tian, Xinmeng; Hu, Jiajia; Chen, Tiantian; Xu, Hui; Yang, GF; Chen, Yanyan] Cent China Normal Univ, Coll Chem, Key Lab Insecticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Xu, H; Yang, GF] C;Cent China Normal Univ, Coll Chem, Key Lab Insecticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Edible biota;Gas chromatography-mass spectrometry;In vivo solid phase microextraction;Insecticide
摘要：
Traditional sample preparation methods for insecticide analysis are laborious and fatal to living organisms. In the work, an in vivo sampling rate calibrated-solid phase microextraction-gas chromatography-mass spectrometry method was established and successfully used for in vivo sampling and quantitative determination of three insecticides (hexachlorobenzene, fipronil and chlorfenapyr) by direct exposing micron-sized fiber in living garlic. Absorption, enrichment, migration and elimination behavior of insecticides in garlic were investigated. Bioaccumulative effects with obvious tissue differences were observed to all three insecticides, especially for chlorfenapyr. Bioconcentration factors (BCFs) ranging from 0.0342 to 1.0887 were obtained, and the closer to roots, the higher BCFs. The half-life of insecticides in garlic ranged from 0.43 to 0.96 d. In the first 24 h, 55.0% − 80.3% insecticides residues in garlic were eliminated with first-order elimination kinetics. The research provides in vivo insights into the environmental fates of insecticides in complex living system with minimized organism damage. © 2021 Elsevier Ltd
语种：
英文
展开
Nitrate promoted defluorination of perfluorooctanoic acid in UV/sulfite system: Coupling hydrated electron/reactive nitrogen species-mediated reduction and oxidation
作者：
Yuan, Yijin;Feng, Lizhen;He, Xianqin;Wu, Mengsi;Ai, Zhihui;...
期刊：
Environmental Pollution ,2022年313:120172 ISSN：0269-7491
通讯作者：
Gong, Jingming(jmgong@mail.ccnu.edu.cn)
作者机构：
[Feng, Lizhen; Zhang, Lizhi; Gong, Jingming; Yuan, Yijin; Wu, Mengsi; He, Xianqin; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Inst Environm & Appl Chem,Minist Educat, Wuhan 430079, Peoples R China.
通讯机构：
[Jingming Gong] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079, PR China
关键词：
Hydrated electron;Integrated oxidation and reduction;Nitrate;Perfluorooctanoic acid;Reactive nitrogen species
摘要：
A significantly accelerated defluorination of recalcitrant perfluorooctanoic acid (PFOA) was explored with the co-present nitrate (20 mg L−1) by UV/sulfite treatment (UV/sulfite-nitrate). The deep defluorination of PFOA and complete denitrification of nitrate were simultaneously achieved in UV/sulfite-nitrate system. At the initial 30 min, PFOA defluorination exhibited an induction period, exactly corresponding to the removal of the co-existed nitrate. Upon the induction period passed, an accelerated removal of PFOA (5 mg L−1) occurred, nearly 100% defluorination ratio reached within 2 h. Compared with those in UV/sulfite, the kinetics of PFOA decay, defluorination, and transformation product formations were greatly enhanced in UV/sulfite-nitrate system. Reactive nitrogen species (RNS) generated from eaq−-induced reduction of nitrate were found to play significant roles on the promoted defluorination apart from eaq−-mediated reductive defluorination. The investigations on solution pH (7.0–11.0) confirmed that the reductive defluorination of PFOA was more efficient under alkaline conditions, however, the presence of nitrate can promote the defluorination even under neutral pH. Theoretical calculations of Fukui function demonstrated that RNS could easily launch electrophilic attack toward H-rich moieties of fluorotelomer carboxylates (FTCAs, CnF2n+1−(CH2)m−COO−), more persistent intermediates (formed via H/F exchange), and convert FTCAs into shorter-chain perfluorinated carboxylic acids, thus facilitating the deep defluorination. Along with the analysis on the denitrification products, the liberation of fluoride ions and generated intermediates, possible decomposition pathways were proposed. This work highlights the indispensable synergy from eaq−/RNS with integrated reduction and oxidation on PFOA defluorination and will advance remediation technologies of perfluorinated compound contaminated water. © 2022 Elsevier Ltd
语种：
英文
展开
Trace Iridium as ″Adhesive″ in PtCuIr Aerogels for Robust Methanol Electrooxidation
作者：
Fang, Qie;Wang, Hengjia;Lv, Xintong;Wei, Xiaoqian;Luo, Xin;...
期刊：
ACS SUSTAINABLE CHEMISTRY & ENGINEERING ,2021年9(38):13039-13046 ISSN：2168-0485
通讯作者：
Song, Weiyu(songwy@cup.edu.cn);Zhu, Chengzhou(czzhu@mail.ccnu.edu.cn)
作者机构：
[Fang, Qie; Huang, Jiajia; Zhu, Chengzhou; Wei, Xiaoqian; Jiao, Lei; Luo, Xin; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Song, Weiyu; Lv, Xintong] China Univ Petr, Coll Sci, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China.
通讯机构：
[Weiyu Song] S;[Chengzhou Zhu] K;State Key Laboratory of Heavy Oil Processing, College of Science, China University of Petroleum-Beijing, Beijing 102249, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P.R. China
关键词：
aerogels;self-assembly;alloys;methanol oxidation reaction;electrocatalysts
摘要：
PtCu-based alloy nanomaterials have shown great potential in methanol oxidation reaction (MOR) owing to the lower cost and good anti-poisoning ability. However, the dissolution of non-precious metal makes them suffer from severe stability issues, greatly impeding the practical application of direct methanol fuel cells. Herein, PtCuIr aerogels are successfully fabricated through a one-step NaBH4reduction strategy to anchor trace Ir on PtCu aerogels based on compositional engineering, which serves as advanced electrocatalysts to achieve enhanced electrocatalytic performance toward MOR. Particularly, the optimized PtCuIr aerogels show extraordinary stability and the mass activity maintains 71.2% of the initial value after 20,000 s chronoamperometric measurements. Density functional theory calculations certify that the doping of trace Ir considerably lowers the adsorption energy of CO-containing substances and thus enhances the MOR activity. By employing the vacancy formation energy of the surface Pt as the descriptor, it is revealed that the robust stability of PtCuIr aerogels originates mainly from the stronger bond between Ir and Pt/Cu atoms, where Ir acts as an ″adhesive″ to prevent the dissolution and leaching of atoms. The breakthrough of the highly stable MOR catalyst could open an avenue for affordable and durable fuel cells. © 2021 American Chemical Society
语种：
英文
展开
Engineering the Redox-Driven Channel for Precisely Regulating Nanoconfined Glutathione Identification and Transport
作者：
Guan, Tianpei;Cheng, Ming;Zeng, Lisi;Chen, Xiaoya;Xie, Yuan;...
期刊：
ACS Applied Materials & Interfaces ,2021年13(41):49137-49145 ISSN：1944-8244
通讯作者：
Wang, Jin;Cui, Shuzhong;Sun, Yao;Li, Haibing
作者机构：
[Lei, Ziying; Wang, Jin; Cui, SZ; Guan, Tianpei; Ruan, Qiang; Cui, Shuzhong; Zeng, Lisi] Guangzhou Med Univ, Dept Gastroentestinal Surg 2, Affiliated Canc Hosp & Inst, Guangzhou 510095, Peoples R China.;[Chen, Xiaoya; Sun, Yao; Sun, Y; Li, Haibing; Cheng, Ming] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Xie, Yuan] Guangdong Prov Key Lab Radioact & Rare Resource U, Shaoguan 512026, Peoples R China.
通讯机构：
[Wang, J; Cui, SZ] G;[Sun, Y; Li, HB] C;Guangzhou Med Univ, Dept Gastroentestinal Surg 2, Affiliated Canc Hosp & Inst, Guangzhou 510095, Peoples R China.;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
artificial intelligent nanochannel;glutathione;host−guest;redox-regulated switch;selective transport
摘要：
Bioinspired artificial nanochannels for molecular and ionic transport have extensive applications. However, it is still a huge challenge to achieve an intelligent transport system with high selectivity/efficiency and controllability. Inspired by glutathione transport across the plasma membrane via redox regulation, we herein designed and fabricated a redox-reactive artificial nanochannel based on the host-guest chemical strategy. The nanochannel platform achieved high selectivity/efficiency for the identification and transmission of glutathione in the confined space. In addition, this nanochannel can switch between the ON and OFF states through the redox reaction. This redox-regulated system can provide a potential application for detection/binding of biological analytes and redox-controlled drug release. © 2021 American Chemical Society.
语种：
英文
展开
PdBi Single-Atom Alloy Aerogels for Efficient Ethanol Oxidation
作者：
Wang, Hengjia;Jiao, Lei;Zheng, Lirong;Fang, Qie;Qin, Ying;...
期刊：
Advanced Functional Materials ,2021年31(38):2103465- ISSN：1616-301X
通讯作者：
Zhu, Chengzhou(czzhu@mail.ccnu.edu.cn);Wen, Jing(jing.wen@wit.edu.cn)
作者机构：
[Fang, Qie; Qin, Ying; Zhu, Chengzhou; Wei, Xiaoqian; Jiao, Lei; Luo, Xin; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Zheng, Lirong] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China.;[Hu, Liuyong; Wen, Jing] Wuhan Inst Technol, Sch Mat Sci & Engn, Wuhan 430205, Peoples R China.
通讯机构：
[Jing Wen] S;[Chengzhou Zhu] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China<&wdkj&>School of Materials Science and Engineering, Wuhan Institute of Technology, Wuhan, 430205 P. R. China
关键词：
aerogels;electrocatalysis;ethanol oxidation reaction;self-assembly;single-atom alloys
摘要：
Single-atom alloys (SAAs) have ignited a surge of unprecedented interest as the advanced nanomaterials and opened many opportunities for wide applications. Herein, 3D porous aerogels comprising ionic liquid (IL) functionalized PdBi SAA building blocks with atomically dispersed Bi on Pd nanowires (IL/Pd50Bi1) are synthesized with accelerated gelation kinetics, which could serve as high-efficiency electrocatalysts for ethanol oxidation reaction (EOR). Benefiting from the unique structures of aerogels including synergistic effects of PdBi SAA nanowire networks and interface engineering, the optimized IL/Pd50Bi1 aerogels display a nearly fourfold enhancement in mass activity and boosted stability for EOR compared to commercial Pd/C. Density functional theory calculations further demonstrate that isolated Bi atoms on Pd nanowire networks decrease the energy barrier of the rate-determining step, resulting in excellent electrocatalytic activity for EOR. This work provides a promising method for developing efficient SAA catalysts for fuel electrooxidation. © 2021 Wiley-VCH GmbH
语种：
英文
展开
