通讯机构：
[Gong, JM ] C;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Ammonia nitrogen;6-Trichlorophenol;Peroxymonosulfate;Dechlorination;Active chlorine species
摘要：
Halogenated phenol and ammonia nitrogen (NH4+-N) are typical composite pollutions in wastewater. It is still unclear how the transformation of halogenated phenol affects the fate of co-existing NH4+-N. In this study, the removal performance of the NH4+-N containing the co-existed halogenated organic, using 2, 4, 6-trichlorophenol (TCP) as the model pollutant was firstly investigated in the waste lithium-ion batteries (LIBs) material-derived catalysts activating peroxymonosulfate system (LIBs/PMS). The rapid degradation of TCP and the selective transformation of NH4+-N to N2 were simultaneously achieved. TCP could be degraded rapidly (within 2 min) whether with or without NH4+-N. Interestingly, the NH4+-N removal was initiated by the co-present TCP, strongly dependent on TCP dechlorination. And NH4+-N removal displayed a thermally accelerated process in the temperature range of 25 to 60 degrees C. With the co-present TCP (60 mg/L), 93.7% of NH4+-N could be removed at 50 degrees C. Based on the capture and the electron spin resonance (ESR) experiments, the generated reactive oxygen species (& BULL;OH, SO4 & BULL; and 1O2) participated in the TCP dechlorination, particularly 1O2 with dominant roles, whereas ClO & BULL; played an important role on NH4+-N removal. Theoretical calculations were used not only to predict the possible reactive site of TCP, but also evaluate the difficulty of reaction between NH4+-N and different active species. Moreover, NH4+-N could be removed 80% in outdoor simulated experiment (in Wuhan) and 100% for chlorobenzene and nitrogen-containing wastewater. This study unveiled the influence of the co-existed halogenated phenol toward the fate of NH4+-N in LIBs/PMS system and enriched the treatment of NH4+-N wastewater strategies.
作者机构：
[Pei, Qijun; Yu, Jiafeng; Qiu, Guanghao; Yu, Yang; Guo, Jianping] Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;[Wen, Junfeng] School of Chemistry and Chemical Engineering, Yulin University, Yulin 719000, China;[Rao, Li] Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China;State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
通讯机构：
[Li Rao] H;Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要：
Liquid organic hydrogen carriers (LOCHs) hold considerable potential for large-scale and long-distance energy/hydrogen storage and transportation. However, due to the lack of efficient catalysts, harsh conditions are needed for the reversible hydrogen uptake and/or release of LOHCs. Herein, a one-pot method was developed to synthesize an ultrafine metastable Ru-B alloy, where the geometrical and electronic structure of Ru is well modulated by B. To our delight, the hydrogenation of N-ethylcarbazole (NEC, one of the promising LOHC candidates) could be catalyzed by Ru-B alloy with ca. 99 % yield to 12H-NEC at room temperature. To the best of our knowledge, this is the first example of realizing the hydrogenation of NEC at room temperature. Theoretical simulations indicate that the (0001) surface of Ru7B3 crystal may be the active site for the catalytic hydrogenation. This work shows the potency of metastable nanomaterials as efficient catalysts for chemical transformations which are kinetically challenging.
作者机构：
[Peng, Hao; Geng, Zi-Qi; Xu, Hao; Qian, Hao-Dong; Li, Si-Jia; Xu, H; Zhao, Chunhui; Peng, H] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr,Key Lab Pesticides & Ch, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构：
[Xu, H ; Peng, H] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr,Key Lab Pesticides & Ch, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
摘要：
The synthesis of chiral triazole-fused pyrazine scaffolds from readily available substrates in a step-economical asymmetric catalytic way is highly appealing. We herein report that an efficient Cu/Ag relay catalyzed protocol employing cascade asymmetric propargylic amination, hydroazidation, and [3 + 2] cycloaddition reaction with high efficiency to access the target enantioenriched 1,2,3-triazolo[1,5-a]pyrazine has been accomplished by applying a novel N,N,P-ligand. The one-pot reaction of three components exhibits high functional group tolerance, excellent enantioselectivities, and a broad substrate scope with readily available starting materials.
作者机构：
[Shen, Baojie; Qi, Yinghua; Chen, Disong; Li, Rui] Cent China Normal Univ, Coll Chem, Lab Mass Spectrometry, Wuhan 430079, Hubei, Peoples R China.;[Zhong, Hongying; Zhong, HY] Guangxi Univ, Coll Life Sci & Technol, Ctr Instrumental Anal, Nanning 530004, Guangxi, Peoples R China.;[Gao, Anji] Chinese Acad Sci, Innovat Acad Precis Measurement Sci & Technol, Wuhan 430071, Peoples R China.;[Gao, Anji] Univ Chinese Acad Sci, Beijing 100049, Peoples R China.
通讯机构：
[Zhong, HY ] G;Guangxi Univ, Coll Life Sci & Technol, Ctr Instrumental Anal, Nanning 530004, Guangxi, Peoples R China.
关键词：
Anaerobic oxidization;Hot electrons;Ligand-bridged electron transfer;Mass spectrometry;Plasmonic nanoreactors
摘要：
The light induced hot-electron on plasmonic nanostructures has been recognized as a breakthrough discovery for photovoltaic and photocatalytic applications. With mass spectrometry, we demonstrate the dynamics of hot electron transfers of anaerobic oxidization reactions on Au decorated TiO2 plasmonic nanoparticles, which were coated on the inner surface of a flask. Those nanoparticles were covered by continuously renewed liquid droplets of solvent and reactants that were transported through a Venturi jet mixer with auto-spray. In addition to intensive mass transfer in such droplet-based nanoreactors, as well as strong adsorption of reactants and rapid desorption of products on materials surfaces, the localized surface plasmon resonance (LSPR) excitation upon visible light illumination, by which accumulated energies of plasmons are transferred to electrons in the conduction band of the material, attributes to the efficient photocatalytic transformation. Mass spectrometric detection of intermediate radical anions and negative ions with stable isotope labeling unambiguously identifies that highly energetic hot electrons can escape from the plasmonic nanostructures, be collected by adsorbed molecules, and initiate bond cleavages. It was demonstrated that losses of two H atoms result in the anaerobic oxidization of each benzyl alcohol molecule to a benzyl aldehyde molecule in the absence of molecular oxygen with more than 90 % yields. The well recyclable plasmonic nanoreactors implicate the injection of transferred electrons eventually back to electronically depleted Au+ positive ions. Bridged by adsorbed molecules, electrons were repeatedly circulated back and forth in plasmonic nanoreactors, where the collected light was eventually converted into chemical energy.
摘要：
LDs (Lipid droplets) are key organelles for lipid metabolism and storage, which are closely related to ferroptosis and fatty liver. Due to its small size and highly dynamic nature, developing high-fidelity fluorescent probes for imaging of LDs is crucial for observing the dynamic physiological processes of LDs and investigating LDs-associated diseases. Herein, we synthesized three dicyanoisophorone-based fluorescent probes (DCIMe, DCIJ, and DCIQ) with different electron-donating groups and studied their imaging performance for LDs. The results show that DCIQ is highly polarity sensitive and can perform high-fidelity imaging for LDs, with significantly better performance than DCIMe, DCIJ, and commercial LD probe BODIPY 493/503. Based on this, DCIQ was successfully applied to real-time observe the interplays between LDs and other organelles (mitochondria, lysosomes, and endoplasmic reticulum), and to image the dynamics of LDs with fast scanning mode (0.44s/frame) and the generation of oleic acid-induced LDs with high-fidelity. Finally, DCIQ was used to study the changes of LDs in the ferroptosis process and nonalcoholic fatty liver disease tissues. Overall, this study provided a powerful tool for high-fidelity imaging of LDs in cells and tissues.
期刊：
Trends in Biochemical Sciences,2023年48(6):539-552 ISSN：0968-0004
通讯作者：
Hao, Ge-Fei;Yang, GF;Hao, GF
作者机构：
[Yang, Guang-Fu; Wang, Zhi-Zheng; Yang, GF; Shi, Xing-Xing; Huang, Guang-Yi; Hao, Ge-Fei] Cent China Normal Univ, Natl Key Lab Green Pesticide, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Hao, Ge-Fei] Guizhou Univ, Ctr R&D Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr BioEngn,Minist Educ, Guiyang 550025, Peoples R China.
通讯机构：
[Hao, GF ] G;[Yang, GF ; Hao, GF] C;Cent China Normal Univ, Natl Key Lab Green Pesticide, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;Guizhou Univ, Ctr R&D Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr BioEngn,Minist Educ, Guiyang 550025, Peoples R China.
关键词：
PPI modulator;fragment evolution;fragment screening;hot spot;structure-based drug design
摘要：
Protein-protein interactions (PPIs) have important roles in various cellular processes, but are commonly described as 'undruggable' therapeutic targets due to their large, flat, featureless interfaces. Fragment-based drug discovery (FBDD) has achieved great success in modulating PPIs, with more than ten compounds in clinical trials. Here, we highlight the progress of FBDD in modulating PPIs for therapeutic development. Targeting hot spots that have essential roles in both fragment binding and PPIs provides a shortcut for the development of PPI modulators via FBDD. We highlight successful cases of cracking the 'undruggable' problems of PPIs using fragment-based approaches. We also introduce new technologies and future trends. Thus, we hope that this review will provide useful guidance for drug discovery targeting PPIs.
期刊：
JOURNAL OF MEDICINAL CHEMISTRY,2023年66(1):371-383 ISSN：0022-2623
通讯作者：
Chuan-Fei Jin<&wdkj&>Ge-Fei Hao
作者机构：
[Nie, Biao; Xue, Ya-Ping; Wang, Zhi-Zheng; Lu, Jie-Lian; Wang, Zu-Sheng; Chen, Kang-Zhi; Zhang, Ying-Jun; Xu, Teng-Fei; Huang, Jun-Jie; Hao, Ge-Fei] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430000, Peoples R China.;[Nie, Biao; Xue, Ya-Ping; Lu, Jie-Lian; Wang, Zu-Sheng; Chen, Kang-Zhi; Zhang, Ying-Jun; Xu, Teng-Fei; Huang, Jun-Jie; Hao, Ge-Fei] Guizhou Univ, Ctr R&D Fine Chem, State Key Lab Breeding Base Green Pesticide & Agr, Key Lab Green Pesticide,Minist Educ, Guiyang 550025, Peoples R China.;[Jin, Chuan-Fei; Yi, Chao] HEC Res & Dev Ctr, HEC Pharm Grp, Dongguan 523871, Peoples R China.;[Nie, Biao; Xue, Ya-Ping; Lu, Jie-Lian; Wang, Zu-Sheng; Chen, Kang-Zhi; Jin, Chuan-Fei; Zhang, Ying-Jun; Xu, Teng-Fei; Huang, Jun-Jie] Sunshine Lake Pharm Co Ltd, Shenzhen 518000, Peoples R China.
通讯机构：
[Chuan-Fei Jin; Ge-Fei Hao] S;State Key Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Key Laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education, Center for R&D of Fine Chemicals, Guizhou University, Guiyang 550025, China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430000, China<&wdkj&>Sunshine Lake Pharma Co. Ltd., Shenzhen 518000, China<&wdkj&>HEC Pharm Group, HEC Research and Development Center, Dongguan 523871, China
摘要：
Inadequate bioavailability is one of the most critical reasons for the failure of oral drug development. However, the way that substructures affect bioavailability remains largely unknown. Serotonin transporter (SERT) inhibitors are first-line drugs for major depression disorder, and improving their bioavailability may be able to decrease side-effects by reducing daily dose. Thus, it is an excellent model to probe the relationship between substructures and bioavailability. Here, we proposed the concept of "nonbioavailable substructures", referring to substructures that are unfavorable to bioavailability. A machine learning model was developed to identify nonbioavailable substructures based on their molecular properties and shows the accuracy of 83.5%. A more potent SERT inhibitor DH4 was discovered with a bioavailability of 83.28% in rats by replacing the nonbioavailable substructure of approved drug vilazodone. DH4 exhibits promising anti-depression efficacy in animal experiments. The concept of nonbioavailable substructures may open up a new venue for the improvement of drug bioavailability.
摘要：
Inefficient usage, overdose, and post-application losses of conventional pesticides have resulted in severe ecological and environmental issues, such as pesticide resistance, environmental contamination, and soil degradation. Advances in nano-based smart formulations are promising novel methods to decrease the hazardous impacts of pesticide on the environment. In light of the lack of a systematic and critical summary of these aspects, this work has been structured to critically assess the roles and specific mechanisms of smart nanoformulations (NFs) in mitigating the adverse impacts of pesticide on the environment, along with an evaluation of their final environmental fate, safety, and application prospects. Our study provides a novel perspective for a better understanding of the potential functions of smart NFs in reducing environmental pollution. Additionally, this study offers meaningful information for the safe and effective use of these nanoproducts in field applications in the near future.
关键词：
CO2 Reduction;Dual-Single-Atom Catalyst;Electronic Interaction;Reaction Mechanism;Solar
摘要：
Solar‐to‐chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO2 reduction. Herein, a new concentrated solar‐driven photothermal system coupling a dual‐metal single‐atom catalyst (DSAC) with adjacent Ni‐N4 and Fe‐N4 pair sites is designed for boosting gas‐solid CO2 reduction with H2O under simulated solar irradiation even ambient sunlight. As expected, the (Ni, Fe)‐N‐C DSAC exhibits a superior photothermal catalytic performance for CO2 reduction to main CO (86.16 μmol g−1 h−1), CH4 (135.35 µmol g−1 h−1) and CH3OH (59.81 µmol g−1 h−1) productions, which are equivalent to 1.70‐fold, 1.27‐fold and 1.23‐fold higher than those of Fe‐N‐C catalyst, respectively. Based on theoretical simulations, the Fermi level and d‐band center of Fe atom is efficiently regulated in non‐interacted Ni and Fe dual‐atom pair sites with electronic interaction through electron orbital hybridization on (Ni, Fe)‐N‐C DSAC. Crucially, the spatially proper distance between adjacent Ni and Fe atoms of Ni‐N‐N‐Fe configuration induces that the additional Ni atom as a new active site contribute to the main *COOH and *HCO3 dissociation to optimize the corresponding energy barriers in the reaction process, leading to specific dual reaction pathways (COOH and HCO3 pathways) for solar‐driven photothermal CO2 reduction to initial CO production.
期刊：
Energy Storage Materials,2023年63 ISSN：2405-8297
通讯作者：
Mai, LQ;Guo, YB;Luo, W
作者机构：
[Feng, Wencong; Yu, Ruohan; Mai, Liqiang; Shen, Chunli; Wang, Junjun; Wang, Hong; Cheng, Chaojie; Xv, Xianmin] Wuhan Univ Technol, Sch Mat Sci & Engn, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;[Guo, Yanbing; Guo, YB; Zhang, Biluan; Pan, Chuanqi] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Yu, Ruohan; Wang, Hong] Wuhan Univ Technol, Nanostruct Res Ctr NRC, Wuhan 430070, Peoples R China.;[Luo, Wen] Wuhan Univ Technol, Sch Sci, Dept Phys, Wuhan 430070, Peoples R China.;[Guo, Yanbing] Minist Educ, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Wuhan 430079, Peoples R China.
通讯机构：
[Guo, YB ] C;[Luo, W ; Mai, LQ ] W;Wuhan Univ Technol, Sch Mat Sci & Engn, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;Wuhan Univ Technol, Sch Sci, Dept Phys, Wuhan 430070, Peoples R China.
关键词：
Self-regulating ion -transport channels;Graphdiyne;Potassium-ion batteries;in situ TEM and Raman;Molecular carbon skeleton
摘要：
Developing anode materials with multiple-dimensional ion transport channels, especially to overcome huge volume expansion and sluggish ion diffusion kinetics caused by large radius of potassium ion (K+), is critical to improve the potassium storage performance. Herein, we propose a self-reversible conversion of chemical bonds with different bond lengths based on graphdiyne (GDY) to self-regulating the ion transport channels. Density functional theory (DFT) calculations and ex/in situ electrochemical tests proof the in-plane triangular-like pores (5.46 angstrom) of the GDY framework offer a transport channel for K+ (1.38 angstrom) diffusion in the direction perpendicular to the GDY plane, which differs it from carbonaceous materials whose ion diffusion is mostly governed by in-plane migration. Furthermore, the reversible alkyne-alkene bonds linking/breaking of GDY stimulated by K+ to realize self-regulating ion channels are demonstrated by in situ Raman and electro-kinetic analysis. Moreover, compared to graphite, the GDY anode with 2 orders of magnitude diffusion coefficient delivered a high reversible capacity of 202 mAh g- 1 at 100 mA g- 1 exhibited extraordinary durability corresponding to cycle time over 380 days. This work opens a new avenue of designing intelligent, efficient ion transport channels from molecular carbon skeleton perspective to enhance diffusion kinetic for high-performance KIBs.
摘要：
Semiconductor-based photoelectrochemical (PEC) biosensors have garnered significant attention in the field of disease diagnosis and treatment. However, the recognition units of these biosensors are mainly limited to bioactive macromolecules, which hinder the photoelectric response due to their insulating characteristics. In this study, we develop an in situ-sensitized strategy that utilizes a small-molecule probe at the interface of the photoelectrode to accurately detect α-glucosidase (α-Glu) activity. Silane, a prototype small-molecule probe, was surface-modified on graphitic carbon nitride to generate Si nanoparticles upon reacting with hydroquinone, the enzymatic product of α-Glu. The in situ formed heterojunction enhances the light-harvesting property and photoexcited carrier separation efficiency. As a result, the in situ-sensitized PEC biosensor demonstrates excellent accuracy, a low detection limit, and outstanding anti-interference ability, showing good applicability in evaluating α-Glu activity and its inhibitors in human serum samples. This novel in situ sensitization approach using small-molecule probes opens up new avenues for developing simple and efficient PEC biosensing platforms by replacing conventional biorecognition elements.
摘要：
A unique photoelectrochemical fuel cell consisting of dual photoelectrodes is developed by utilizing light, ascorbic acid, and oxygen to produce electric power. Specifically, the integration of bifunctional single‐atom iron cocatalysts significantly facilitates anodic ascorbic acid oxidation reaction and cathodic oxygen reduction reaction, effectively improving interfacial reaction kinetics and photoelectric conversion efficiency. Abstract Semiconductor‐based photoelectrochemical (PEC) fuel cells offer a feasible solution for sustainable and environmentally friendly energy production by converting solar and chemical energy into electrical energy. However, the low PEC activities of PEC fuel cells have hindered their practical application due to rapid electron‐hole recombination and slow interfacial reaction kinetics. To address this issue, a unique PEC fuel cell composed of dual photoelectrodes utilizing low‐cost biomass, ascorbic acid, as an organic fuel is reported. Significantly, the integration of bifunctional iron single‐atom catalysts (Fe SACs) and photoactive materials has effectively constructed a bridge for charge carrier transfer, boosting interfacial reaction kinetics and photoelectric conversion efficiency. Notably, the optimal dual‐photoelectrode PEC fuel cell decorated with Fe SACs exhibits superior performance, delivering a maximum power density of 82.82 µW cm−2. Taking advantage of the peroxidase‐like activity of Fe SACs, the resultant self‐powered PEC fuel cells are explored for sensitively detecting actual uric acid samples. This study provides a promising avenue to boost the energy conversion efficiency of PEC fuel cells for sensitive self‐powered biosensing.
摘要：
Mimicking the structure of natural enzymes for designing advanced alternatives provides great opportunities to address the bottleneck of enzyme-involved chemiluminescence (CL). Herein, according to theoretical calculations, we found that an endogenous axial ligand of M-N-C single-atom nanozymes (SAzymes), originating from OH- spontaneously bonding to the metal center in an alkaline medium, can self-adaptively change its strength to facilitate intermediate steps. Furthermore, the lowest energy barrier of the rate-determining step and the strongest affinity and fastest electron transfer with luminol anion endow Co-N-C with the highest peroxidase-like activity. Guided by the theoretical calculations, a series of M-N-C SAzymes (M=Fe, Co, Ni) were synthesized to boost CL, where Co-N-C SAzymes with superior catalytic activity and high selective generation of O(2)(center dot-)were validated. As a proof-of-concept, Co-N-C SAzymes were employed for sensitive detection of acetylcholinesterase and organophosphorus pesticide.
作者机构：
[Xu, Weiqing; Fang, Qie; Tang, Yinjun; Zhu, Chengzhou; Wei, Xiaoqian; Zhu, CZ; Luo, Xin; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Hubei Engn Technol Res Ctr Optoelect & New Energy, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.
通讯机构：
[Zhu, CZ ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
Developing functional nanomaterials for nonenzymatic glucose electrochemical sensing platforms is vital and challenging from the perspective of pathology and physiology. Accurate identification of active sites and thorough investigation of catalytic mechanisms are critical prerequisites for the design of advanced catalysts for electrochemical sensing. Herein, Cu aerogels are synthesized as a model system for sensitive nonenzymatic glucose sensing. The resultant Cu aerogels exhibit good catalytic activity for glucose electrooxidation with high sensitivity and a low detection limit. Significantly, in situ electrochemical investigations and Raman characterizations reveal the catalytic mechanism of Cu-based nonenzymatic glucose sensing. During the electrocatalytic oxidation of glucose, Cu(I) is electrochemically oxidized to generate Cu(II), and the resultant Cu(II) is spontaneously reduced back to Cu(I) by glucose, achieving the sustained Cu(I)/Cu(II) redox cycles. This study provides profound insights into the catalytic mechanism for nonenzymatic glucose sensing, which provides great potential guidance for a rational design of advanced catalysts in the future.
作者机构：
[Qin, Ying; Tang, Yinjun; Zhu, Chengzhou; Li, Jinli; Jiao, Lei; Gu, Wenling; Fang, Qie; Liu, Mingwang; Wu, Yu] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Wen, Jing; Hu, Liuyong] Wuhan Inst Technol, Hubei Engn Technol Res Ctr Optoelect & New Energy, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.;[Zheng, Lirong; Cui, Xiaowen] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China.;[Guo, Shaojun] Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China.
通讯机构：
[Chengzhou Zhu] N;[Liuyong Hu] H;[Shaojun Guo] S;National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, China<&wdkj&>Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials, Wuhan Institute of Technology, Wuhan, China<&wdkj&>School of Materials Science and Engineering, Peking University, Beijing, China
摘要：
Carrier migration path and driving forces are two crucial factors for charge separation of heterojunction with efficient photoelectric response from the thermodynamic and kinetic perspectives, respectively. Constructing the S-scheme heterojunction and achieving an efficient migration path for space charge separation have aroused great interest, while a thorough insight into tuning interfacial band bending for S-scheme heterojunction is absent. Herein, we report a class of Zn atom-doped CeO2/g-C3N4 heterostructure for achieving a new carrier migration path conversion from inferior type-II to advanced S-scheme. Zn-dependent volcano-type plot for Zn-CeO2 is established to tune the Fermi level of CeO2. The built-in electric field for carrier flow dynamics strengthens when coupling with g-C3N4, which significantly boosts the photoelectric response. Based on the intrinsic enzymelike activity of Zn-CeO2, we further demonstrate that the Zn-CeO2/g-C3N4 S-scheme heterojunction can be explored for constructing a sensitive nanozymatic photoelectrochemical biosensor for the detection of acetylcholinesterase.
作者机构：
[Xu, Weiqing; Tang, Yinjun; Luo, Zhen; Zhu, Chengzhou; Song, Weiyu] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Guo, Shaojun] Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China.;[Chen, Yanjun; Song, Weiyu] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China.;[Ye, Hua-Rong] Wuhan Univ Sci & Technol, China Resources & Wisco Gen Hosp, Dept Med Ultrasound, Wuhan 430079, Peoples R China.
通讯机构：
[Shaojun Guo] S;[Chengzhou Zhu] K;School of Materials Science and Engineering, Peking University, Beijing 100871, P. R. 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
摘要：
Great efforts have been made to expand the application fields of nanozymes, which puts forward requirements for nanozymes with both superior catalytic activity and specificity. Herein, we reported the high-indexed intermetallic Pt(3)Sn (H-Pt(3)Sn) with high peroxidase-like activity and specificity. The resultant H-Pt(3)Sn exhibits a specific activity of 345.3 U/mg, which is 1.82 times higher than Pt. Moreover, H-Pt(3)Sn possesses negligible oxidase-like and catalase-like activities, achieving superior catalytic specificity toward H(2)O(2) activation. Experimental and theoretical calculations reveal both the splitting energy for adsorbed H(2)O(2) and the energy barrier for the rate-determining step of H-Pt(3)Sn are significantly decreased compared with Pt(3)Sn and Pt. Finally, a nanozyme-linked immunosorbent assay is successfully developed, achieving the sensitive and accurate colorimetric detection for carcinoembryonic antigen with a low detection limit of 0.49 pg/mL and showing practical feasibility in serum sample detection.
通讯机构：
[Tingjuan Gao; Lizhi Zhang] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Institute of Environmental Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Institute of Environmental Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
关键词：
In-situ remediation dynamics;Petroleum contaminants;Raman spectroscopy and microscopy;Soil and groundwater
摘要：
The mechanistic study of soil and groundwater remediation in petroleum contaminated lands significantly demands rapid qualitative and quantitative identification of petroleum substances. However, most traditional detection methods cannot provide the on-site or in-situ information of petroleum compositions and contents simultaneously even with multi-spot sampling and complex sample preparation. In this work, we developed a strategy for the on-site detection of petroleum compositions and in-situ monitoring of petroleum contents in soil and groundwater using dual-excitation Raman spectroscopy and microscopy. The detection time was 0.5h for the Extraction-Raman spectroscopy method and one minute for the Fiber-Raman spectroscopy method. The limit of detection was 94ppm for the soil samples and 0.46ppm for the groundwater samples. Meanwhile, the petroleum changes at the soil-groundwater interface were successfully observed by Raman microscopy during the in-situ chemical oxidation remediation processes. The results revealed that hydrogen peroxide oxidation released petroleum from the interior to the surface of soil particles and then to groundwater during the remediation process, while persulfate oxidation only degraded petroleum on the soil surface and in groundwater. This Raman spectroscopic and microscopic method can shed light on the petroleum degradation mechanism in contaminated lands, and facilitate the selection of suitable soil and groundwater remediation plans.
摘要：
In living organisms, chiral molecules have specific chiral conformations that produce different physiological effects. Ribose is one of the components of RNA, which mainly plays a role in regulating biological activity. Inspired by the biological recognition of sugars, functional chiral surfaces for recognizing L-ribose through non-covalent interactions were constructed. In the strategy of this study, a functional chiral gold surface based on host-guest interactions was constructed through the assembly of the host molecule single-function alynyl pillar[5]arene(SAP5) and the guest molecule (S) -mandelate-violet (SMV). The association constant of SMV and SAP5 was calculated to be 2.95×10(4)M(-1), with a binding ratio of 1:1. By impedance and contact angle detection, the constructed functional interface has good detection effect on L-ribose in the range of 1×10(-7)M to1×10(-2)M. In addition, CV was disassembled from the aromatic cavity of pillar[5]arene after adding zinc powder and it can repeat five times with good recyclability, thus achieving the organic combination of interface recognition and intelligence.
