作者： Luo, Xin;Zhao, Songlin;Luo, Zhen;Li, Shentian;Zhao, Xiao;...

期刊： Chemical Engineering Journal,2023年463:142184 ISSN：1385-8947

通讯作者： Zhu, Zhihong(zhzhu@mail.ccnu.edu.cn)

作者机构： [Zhao, Xiao; Luo, Xin; Li, Shentian] Hubei Univ Technol, Hubei Prov Cooperat Innovat Ctr Ind Fermentat, Natl Ctr Cellular Regulat & Mol Pharmaceut 111, Hubei Res Ctr Food Fermentat Engn & Technol,Key La, Wuhan 430068, Peoples R China.;[Zhu, Zhihong; Zhao, Songlin] Cent China Normal Univ, Inst Nanosci & Nanotechnol, Coll Phys Sci & Technol, Wuhan 430079, Peoples R China.;[Luo, Zhen; Fang, Qie; Wei, Xiaoqian; 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.;[Wang, Canglong] Chinese Acad Sci, Inst Modern Phys, Lanzhou 730000, Peoples R China.

通讯机构： [Zhihong Zhu] I;[Wenling Gu] N;Institute of Nano-science and Nano-technology, College of Physical Science and Technology, Central China Normal University, Wuhan 430079, PR China<&wdkj&>National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, PR China

关键词： Ru;Co nanoparticles;Co-N-C;Carbon nanotube frameworks;Synergistic effect;Oxygen reduction reaction

摘要： The development of metal-nitrogen-codoped carbon catalysts for oxygen reduction reaction (ORR) is highly desired for the practical applications of energy conversion technologies, but there remains a challenge in elucidating mechanisms of structure–activity relationship for enhancing electrocatalytic performance. Herein, we propose a general approach for the synthesis of metallic RuCo nanoparticles and CoNx species embedded in N-doped carbon electrocatalysts (RuCo@Co[sbnd]N[sbnd]C). Benefiting from the synergistic effect of chemical compositions and 3D hierarchical structures, RuCo@Co[sbnd]N[sbnd]C exhibits high ORR activity and superior durability, outperforming Pt/C catalysts. Density functional theory further reveals that Ru@CoNx possesses stronger reactant adsorption ability and a lower dissociation energy barrier than Co@CoNx, which is conducive to accelerating ORR kinetics. Moreover, the Zn-air battery using RuCo@Co[sbnd]N[sbnd]C as the air cathode presents higher power densities, larger specific capacities and stronger cycling stability, outperforming the Pt/C + RuO2 counterparts. This work presents a perspective for the controllable design of highly-efficient electrocatalysts for energy storage applications. © 2023 Elsevier B.V.

语种： 英文

作者： Zhou, Xue-Song;Zhang, Zhihan;Qu, Wen-Yuan;Liu, Xiao-Peng;Xiao, Wen-Jing*;...

期刊： JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2023年145(22):12233-12243 ISSN：0002-7863

通讯作者： Xiao, Wen-Jing;Chen, JR;Jiang, M;Xiao, WJ

作者机构： [Qu, Wen-Yuan; Xiao, Wen-Jing; Chen, Jia-Rong; Zhou, Xue-Song; Liu, Xiao-Peng; Xiao, WJ; Zhang, Zhihan; Chen, JR] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Jiang, Min] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Hangzhou 310036, Zhejiang, Peoples R China.;[Xiao, Wen-Jing; Chen, Jia-Rong; Xiao, WJ; Chen, JR] Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.;[Xiao, Wen-Jing; Xiao, WJ] Shanghai Inst Organ Chem, State Key Lab Organometall Chem, Shanghai 200032, Peoples R China.;[Chen, Jia-Rong; Chen, JR] Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Peoples R China.

通讯机构： [Jiang, M ] H;[Xiao, WJ ] S;[Xiao, WJ; Chen, JR ] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Hangzhou 310036, Zhejiang, Peoples R China.

摘要： Photocatalytic [3 + 2] cycloadditions and control of stereochemistry have remained a substantial challenge, particularly in the context of heterocycle synthesis; sporadic successful examples have involved enantioselective [3 + 2] photocycloaddition between redox-active direct group-containing cyclopropanes and alkenes for creation of cyclopentanes. Herein, we report a cooperative catalytic system comprising a chiral nickel Lewis acid catalyst and an organic photocatalyst fueled by visible-light irradiation that allows for the hitherto elusive asymmetric [3 + 2] photocycloaddition of β-keto esters with vinyl azides under redox-neutral conditions. This protocol enables highly enantioselective construction of polycyclic densely substituted 3,4-dihydro-2H-pyrrole heterocycles featuring two contiguous tetrasubstituted carbon stereocenters, including a useful chiral N,O-ketal motif that is not easily accessible with other catalytic methods. Mechanistic studies revealed that the overall reactivity relies on the seamless integration of dual roles of nickel catalysts by the catalytic formation of the substrate/Ni complex, assisting both photoredox event and enantioselective radical addition. © 2023 American Chemical Society. All rights reserved.

语种： 英文

作者： Li, Ao;Wu, Mengling;Zhang, Junle;Song, Fahui;Pan, Fangfang

期刊： DALTON TRANSACTIONS,2023年52(16):5065-5074 ISSN：1477-9226

通讯作者： Song, Fahui(ffpan@ccnu.edu.cn);Pan, Fangfang(ffpan@ccnu.edu.cn)

作者机构： [Li, Ao; Pan, Fangfang; Wu, Mengling; Song, Fahui] Cent China Normal Univ, Coll Chem, Key Lab Pesticides,Key Lab Pesticides & Chem Biol,, uOttawa Joint Res Ctr,Hubei Int Sci & Technol Coo, Wuhan 430079, Hubei, Peoples R China.;[Zhang, Junle] Huanghe Sci & Technol Univ, Fac Engn, Zhengzhou 450061, Henan, Peoples R China.

通讯机构： [Li, Ao] C;CCNU-uOttawa Joint Research Centre, Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, Key Laboratory of Pesticides & Chemical Biology Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, Hubei, People's Republic of China.

摘要： Successive structural transformations were observed in a methanolic solution containing 4-iodo-1-methylpyridin-1-ium iodide (IPyMe·I) and bismuth iodide (BiI3). When kept in the solution, the amorphous solid (P_1) obtained immediately on mixing would transform to needle crystals (C_1) in hours, which would convert to prismatic crystals (C_2) in around 2 days. In the presence of hydroiodic acid, the hydrothermal reaction of IPyMe·I and BiI3 also gave rise to C_2, and crystals of C_2 in this solution would transform to a third crystalline product C_3 in ca. 3 days. X-ray single crystal diffraction experiments show C_1 containing one-dimensional {BiI4−}n chains, C_2 as a binuclear Bi2I93− structure, and C_3 consisting of a monomeric BiI63− unit, all with IPyMe+ as counter cations. Halogen bonds exist between IPyMe+ and the iodobismuthate, which may play key roles in the structural transformation. By introducing halogen bonding, the hybrids demonstrate excellent water-resistance. A thermal-induced reversible colour change from yellow to dark red occurred from 100 K to 450 K for all three hybrids, in which lattice expansion over the temperature range may be a reason for the thermochromism. The bandgaps derived from the UV-vis diffusion reflectance for the three complexes were 1.80 eV for C_1, 1.84 eV for C_2 and 2.00 eV for C_3. DTF computations followed by electron density topological analysis were applied to explain the structure-optical property relationship for complexes of diverse iodobismuthate types but the same counter cation. It was found that the nature of the Bi-I bonds rather than the dimensionality of the inorganic iodobismuthates is mainly responsible for the light absorption of the materials. © 2023 The Royal Society of Chemistry.

语种： 英文

作者： Tu, Le;Li, Chonglu;Xiong, Xiaoxing;Kim, Ji Hyeon;Li, Qian;...

期刊： ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023年62(15):e202301560- ISSN：1433-7851

通讯作者： Sun, Yao(sunyaogbasp@ccnu.edu.cn);Seung Kim, Jong(jongskim@korea.ac.kr)

作者机构： [Tu, Le; Mei, Longcan; Li, Junrong; Sun, Yao; Li, Chonglu] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Xiong, Xiaoxing] Wuhan Univ, Dept Neurosurg, Renmin Hosp, Wuhan 430060, Peoples R China.;[Kim, Jong Seung; Kim, Ji Hyeon] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Li, Qian] Qingdao Univ Sci & Technol, Key Lab Opt Elect Sensing & Analyt Chem Life Sci, Qingdao 266100, Peoples R China.;[Liu, Shuang] Wuhan Univ Technol, Sch Mat Sci & Engn, Wuhan 430070, Peoples R China.

通讯机构： [Prof. Jong Seung Kim] D;[Prof. Yao Sun] N;National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079 China<&wdkj&>Department of Chemistry, Korea University, Seoul, 02841 Korea

关键词： Anticancer;Molecular Engineering;Photodynamic Therapy;RuII Metallacycle;Supramolecular Chemistry

摘要： Although metallacycle‐based supramolecular photosensitizers (PSs) attracted increasing attention in biomedicine, their clinical translation is still hindered by their inherent dark toxicity. Herein, we report what to our knowledge is the first example of a molecular engineering approach to building blocks of metallacycles for constructing a series of supramolecular PSs (RuA–RuD), with the aim of simultaneously reducing dark toxicity and enhancing phototoxicity, and consequently obtaining high phototoxicity indexes (PI). Detailed in vitro investigations demonstrate that RuA–RuD displays high cancer cellular uptake and remarkable antitumor activity even under hypoxic conditions. Notably, RuD exhibited no dark toxicity and displayed the highest PI value (~406). Theoretical calculations verified that RuD has the largest steric hindrance and the lowest singlet‐triplet energy gap (ΔEST, 0.61 eV). Further in vivo studies confirmed that RuD allows for safe and effective phototherapy against A549 tumors.

语种： 英文

作者： Zhang, Shoute;Meng, Ying;Kemp, K. Christian;Pan, Chuanqi;Ding, Qianzhao;...

期刊： Chemical Engineering Journal,2023年452:139143 ISSN：1385-8947

通讯作者： Li, T

作者机构： [Li, T; Meng, Ying; Li, Tao; Zhang, Shoute; Ding, Qianzhao] Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Hubei Key Lab Mat Chem & Serv Failure, Sch Chem & Chem Engn,Minist Educ, Wuhan 430074, Peoples R China.;[Kemp, K. Christian] POSTECH, Div Environm Sci & Engn, Ctr Ordered Nanoporous Mat Synth, Pohang 37673, South Korea.;[Pan, Chuanqi] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Peoples R China.;[Pang, Lei] DongFeng Trucks R&D Ctr, Zhushanhu Rd 653, Wuhan 430056, Peoples R China.;[Cai, Weiquan] Guangzhou Univ, Guangzhou Higher Educ Mega Ctr, Sch Chem & Chem Engn, 230 Wai Huan Xi Rd, Guangzhou 510006, Peoples R China.

通讯机构： [Li, T ] H;Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Hubei Key Lab Mat Chem & Serv Failure, Sch Chem & Chem Engn,Minist Educ, Wuhan 430074, Peoples R China.

关键词： Cu-SAPO-34;Hydrothermal stability;NH3-SCR;Protective mechanisms

摘要： The low-temperature hydrothermal instability of Cu-SAPO-34 is an unresolved issue, thus jeopardizing its commercial application in NH3-SCR due to severe structural damage and loss of activity. Herein, we reported that efficient strategies i.e., rare earth metal (REM, denotes Ce, La, and Sm) incorporation, alkali metal (AM, denotes Na, K, and Cs) exchange, and NH3 pre-adsorption were utilized to boost the moisture stability of Cu-SAPO-34 through various protective mechanisms. Our extensive characterizations revealed that AM ions readily exchanged with the susceptive Si–O(H)–Al bonds and ZCu(OH) sites, and at the same time left a majority of undamaged Z2Cu sites providing optimal protective effect in the entire temperature window studied here. On the other hand, REM co-cations only guarded Si–O(H)–Al bonds and Z2Cu sites but not the ZCu(OH) sites, this resulted in a poor protective effect in the low-temperature region. By contrast, chemisorbed NH3 only partially prevented Si–O(H)–Al and ZCu(OH) sites from hydrolysis, explaining why this protective effect was superior to REM in the low-temperature region but inferior to REM in the high-temperature region. These different protective mechanisms were explicitly revealed and were used in combination for the first time showing that the hydrothermal stability of Cu-SAPO-34 could be tuned precisely, the mechanistic guidance given here will surely be useful in developing more durable SCR catalysts. © 2022

语种： 英文

作者： Li, Chonglu;Tu, Le;Yang, Jingfang;Liu, Chang;Xu, Yuling;...

期刊： CHEMICAL SCIENCE,2023年14(11):2901-2909 ISSN：2041-6520

通讯作者： Sun, Yan(elaine.sun@utah.edu);Stang, Peter J.(stang@chem.utah.edu);Sun, Yao(sunyaogbasp@ccnu.edu.cn)

作者机构： [Xu, Yuling; Tu, Le; Li, Junrong; Sun, Yao; Li, Chonglu; Yang, Jingfang; Liu, Chang] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Tuo, Wei; Sun, Yan] Henan Univ, Minist Educ, Key Lab Special Funct Mat, Kaifeng 475004, Peoples R China.;[Stang, Peter J.; Tuo, Wei] Univ Utah, Dept Chem, Salt Lake City, UT 84112 USA.;[Olenyuk, Bogdan] Proteogen Res Inst Syst Med, 505 Coast Blvd South, La Jolla, CA 92037 USA.

通讯机构： [Tuo, Wei] M;[Tuo, Wei] D;[Li, Chonglu] N;National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensor Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>Department of Chemistry, University of Utah, Salt Lake City, Utah 84112, USA<&wdkj&>Ministry of Education Key Laboratory for Special Functional Materials, Henan University, Kaifeng 475004, China

摘要： Although metallacycle-based photosensitizers have attracted increasing attention in biomedicine, their clinical application has been hindered by their inherent dark toxicity and unsatisfactory phototherapeutic efficiency. Herein, we employ a π-expansion strategy for ruthenium acceptors to develop a series of Ru(ii) metallacycles (Ru1-Ru4), while simultaneously reducing dark toxicity and enhancing phototoxicity, thus obtaining a high phototoxicity index (PI). These metallacycles enable deep-tissue (∼7 mm) fluorescence imaging and reactive oxygen species (ROS) production and exhibit remarkable anti-tumor activity even under hypoxic conditions. Notably, Ru4 has the lowest dark toxicity, highest ROS generation ability and an optimal PI (∼146). Theoretical calculations verify that Ru4 exhibits the largest steric bulk and the lowest singlet-triplet energy gap (ΔEST, 0.62 eV). In vivo studies confirm that Ru4 allows for effective and safe phototherapy against A549 tumors. This work thus is expected to open a new avenue for the design of high-performance metal-based photosensitizers for potential clinical applications. © 2023 The Royal Society of Chemistry

语种： 英文

作者： Wang, Fanyu;Feng, Yaqin;Wang, Zhongsen;Liu, Yi;Gu, Huayu;...

期刊： Applied Surface Science,2023年624:157127 ISSN：0169-4332

通讯作者： Liu, Xiao(liuxiao71@ccnu.edu.cn)

作者机构： [Gu, Huayu; Feng, Yaqin; Liu, Yi; Wang, Fanyu; Wang, Zhongsen; Liu, Xiao] Cent China Normal Univ, Coll Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Xiao Liu] E;Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, PR China

关键词： Water activation;Oxygen vacancy;Low -Temperature HCHO Oxidation;K plus -doped?-MnO2

摘要： H2O activation plays a crucial role in the oxidation process of HCHO, which can create active hydroxyl to attack HCHO molecules and enhance the catalytic activity. Therefore, the construction of highly active sites for H2O activation to accelerate the reaction rate is required. Herein, we constructed and regulated the surface oxygen vacancies over epsilon-MnO2 with the aid of K doping to activate H2O through a simple hydrothermal method. The role of oxygen vacancy produced by K+ doping for H2O activation in HCHO removal was investigated by various technologies, including XPS, TPD, TPSR, and in-situ DRIFTS. It was found that the addition of K+ not only increased the adsorption sites for negatively charged oxygen atoms of HCHO but also provided oxygen vacancies to induce more active hydroxyl species from water activation. The optimal K+-doped epsilon-MnO2 significantly removed 90% of HCHO at 74 degrees C (GHSV = 120 L/g.h, HCHO = 70 ppm). After the stability test at 65 and 80 degrees C for 100 h respectively, the conversion did not show a downward trend. This work innovatively developed a K-doped epsilon-MnO2 catalyst with surface oxygen vacancy to activate H2O and revealed the role of K+ and oxygen vacancy for efficient HCHO oxidation.

语种： 英文

作者： Han, Xin;Guo, Chenxing;Xu, Chen;Shi, Linlin;Liu, Binghui;...

期刊： ACS Nano,2023年17(4):3723–3736 ISSN：1936-0851

通讯作者： Wang, Heng(hengwang@szu.edu.cn);Hao, Xin-Qi(xqhao@zzu.edu.cn);Song, Mao-Ping(mpsong@zzu.edu.cn);Li, Xiaopeng(xiaopengli@szu.edu.cn)

作者机构： [Hao, Xin-Qi; Zhu, Xinju; Song, Mao-Ping; Han, Xin; Liu, Binghui; Shi, Linlin] Zhengzhou Univ, Coll Chem, Green Catalysis Ctr, Zhengzhou 450001, Henan, Peoples R China.;[Lu, Shuai; Wang, Heng; Han, Xin; Guo, Chenxing; Li, Xiaopeng] Shenzhen Univ, Coll Chem & Environm Engn, Shenzhen 518055, Guangdong, Peoples R China.;[Guo, Chenxing] Shenzhen Univ, Sch Biomed Engn, Shenzhen 518060, Guangdong, Peoples R China.;[Xu, Chen] Jiangsu Univ Sci & Technol, Sch Environm & Chem Engn, Zhenjiang 212003, Jiangsu, Peoples R China.;[Zhang, Zhe; Bai, Qixia] Guangzhou Univ, Inst Environm Res Greater Bay Area, Key Lab Water Qual & Conservat Pearl River Delta, Minist Educ, Guangzhou 510006, Guangdong, Peoples R China.

通讯机构： [Heng Wang; Xiaopeng Li] C;[Xin-Qi Hao; Mao-Ping Song] G;Green Catalysis Center, College of Chemistry, Zhengzhou University, Zhengzhou, Henan 450001, China<&wdkj&>College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong 518055, China

关键词： self-assembly;water-soluble metallo-supramolecular cages;nanoreactors;photochemical cross-coupling reactions;supramolecular catalysis

摘要： Water-soluble metallo-supramolecular cages with well-defined nanosized cavities have a wide range of functions and applications. Herein, we design and synthesize two series of metallo-supramolecular octahedral cages based on the self-assembly of two congeneric truxene-derived tripyridyl ligands modified with two polyethylene glycol (PEG) chains, i.e., monodispersed tetraethylene glycol (TEG) and polydispersed PEG-1000, with four divalent transition metals (i.e., Pd, Cu, Ni, and Zn). The resulting monodispersed cages C1-C4 are fully characterized by electrospray ionization mass spectrometry (ESI-MS), nuclear magnetic resonance (NMR) spectroscopy, and single-crystal X-ray diffraction. The polydispersed cages C5-C8 display good water solubilities and can act as nanoreactors to mediate visible-light-promoted C(sp3)-C(sp2) cross-dehydrogenative coupling reactions in an aqueous phase. In particular, the most robust Pd(II)-linked water-soluble polydispersed nanoreactor C5 is characterized by ESI-MS and capable of mediating the reactions with the highest efficiencies. Detailed host-guest binding studies in conjunction with control studies suggest that these cages could encapsulate the substrates simultaneously inside its hydrophobic cavity while interacting with the photosensitizer (i.e., eosin Y). © 2023 American Chemical Society.

语种： 英文

作者： Ruan, Mei-Ling;Liu, Yungen;Zhang, Chunlei;Mao, Xiaowen;Hu, Di;...

期刊： Chemical Communications,2023年59(19):2747-2750 ISSN：1359-7345

通讯作者： Lok, Chun-Nam(cnlok@hku.hk);Che, Chi-Ming(cmche@hku.hk)

作者机构： [Ruan, Mei-Ling] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Che, Chi-Ming; Hu, Di; Lok, Chun-Nam; Zhang, Chunlei; Ruan, Mei-Ling] Univ Hong Kong, State Key Lab Synthet Chem, Pokfulam Rd, Hong Kong, Peoples R China.;[Che, Chi-Ming; Hu, Di; Lok, Chun-Nam; Zhang, Chunlei; Ruan, Mei-Ling] Univ Hong Kong, Dept Chem, P, R China, Pokfulam Rd, Hong Kong, Peoples R China.;[Che, Chi-Ming; Hu, Di; Lok, Chun-Nam; Zhang, Chunlei; Ruan, Mei-Ling] Lab Synthet Chem, Hong Kong Sci Pk, Hong Kong, Peoples R China.;[Che, Chi-Ming; Hu, Di; Lok, Chun-Nam; Zhang, Chunlei; Ruan, Mei-Ling] Chem Biol Ltd, Hong Kong Sci Pk, Hong Kong, Peoples R China.

通讯机构： [Chun-Nam Lok; Chi-Ming Che] S;State Key Laboratory of Synthetic Chemistry, and Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong, P. R. China<&wdkj&>Laboratory for Synthetic Chemistry and Chemical Biology Limited, Hong Kong Science Park, Shatin, Hong Kong, P. R. China<&wdkj&>Department of Chemistry, Southern University of Science and Technology, Shenzhen, Guangdong, P. R. China<&wdkj&>State Key Laboratory of Synthetic Chemistry, and Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong, P. R. China<&wdkj&>Laboratory for Synthetic Chemistry and Chemical Biology Limited, Hong Kong Science Park, Shatin, Hong Kong, P. R. China

摘要： Dihydroartemisinin non-covalently binds liver fatty acid binding protein (FABP1) with micromolar affinity, acts as a FABP1-dependent peroxisome proliferator-activated receptor alpha agonist and inhibits metastatic hepatocellular carcinoma growth.

语种： 英文

作者： Jia, Shanshan;Li, Shu;Gao, Anji;Shen, Baojie;Zhong, Hongying

期刊： Analytical Chemistry,2023年95(13):5575-5584 ISSN：0003-2700

通讯作者： Zhong, Hongying(hyzhong@gxu.edu.cn)

作者机构： [Shen, Baojie; Zhong, Hongying; Li, Shu; Jia, Shanshan] Cent China Normal Univ, Coll Chem, Lab Mass Spectrometry, Key Lab Pesticides & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Zhong, Hongying] Guangxi Univ, Coll Life Sci & Technol, Ctr Instrumental Anal, State Key Lab Conservat & Utilizat Subtrop Agrobio, Nanning 530004, Guangxi, Peoples R China.;[Gao, Anji] Chinese Acad Sci, Innovat Acad Precis Measurement Sci & Technol, Wuhan 430071, Peoples R China.

通讯机构： [Hongying Zhong] S;State Key Laboratory for Conservation and Utilization of Subtropical Agro-Bioresources, Center for Instrumental Analysis of Guangxi University, College of Life Science and Technology, Guangxi University, Nanning, Guangxi 530004, P. R. China<&wdkj&>Laboratory of Mass Spectrometry, College of Chemistry, Key Laboratory of Pesticides and Chemical Biology, Ministry of Education, Central China Normal University, Wuhan, Hubei 430079, P. R. China

摘要： Metal ions on surfaces of various materials as bulk matrices, doped structural units, or functionalized active sites play critical roles in the establishment of physical and chemical properties. Characterization of surface-bound metal ions and metal ion-coupled electron transfer are urgently needed for the determination of material structures as well as for understanding the relationship to macroscopic properties and technological applications. We present here a mass spectrometric (MS) technique that allows the monitoring of metal ion-coupled electron transfer along with spatial distributions, identities, quantities, valences, redox activities, and associated anions. It is based on the coordination of metal ions with chelators that are redox/photo active. Upon the irradiation of a focused laser beam, metal ions on material surfaces that are covered with chelators are evaporated, ionized, and detected with MS. This technique clearly reveals ligand-metal/metal-ligand and ligand-bridged electron transfers through MS or tandem MS/MS experiments. MS images of metal ions on material surfaces with the spatial resolution down to the sub-micrometer level have been obtained. It has been applied to the monitoring of hot electron transfer, leftover positive metal ions in localized surface plasmon resonance, and photocatalytic activities of crystalline facets of TiO2 © 2023 American Chemical Society.

语种： 英文

作者： Liu, Yi;Hu, Haolu;Zheng, Jiamin;Xie, Fei;Gu, Huayu;...

期刊： Applied Catalysis B: Environmental,2023年330:122649 ISSN：0926-3373

通讯作者： Pan, Fangfang;Liu, X;Rostamnia, S

作者机构： [Zheng, Jiamin; Gu, Huayu; Zhang, Lizhi; Hu, Haolu; Liu, Yi; Xie, Fei; Pan, Fangfang; Liu, Xiao] Cent China Normal Univ, 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.;[Rostamnia, Sadegh] Iran Univ Sci & Technol, Dept Chem, Organ & Nano Grp, Tehran 1684613114, Iran.

通讯机构： [Pan, FF; Liu, X ] C;[Rostamnia, S ] I;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;Iran Univ Sci & Technol, Dept Chem, Organ & Nano Grp, Tehran 1684613114, Iran.

关键词： Mullite SmMn2O5;Lattice oxygen activation;Propane oxidation;Interface regulation;Electron transfer

摘要： Surface lattice oxygen (Olatt) over transition metal oxides plays a pivotal role in catalytic combustion of automobile exhaust. The insufficient Olatt activity at low temperatures, however, remains the key problem restricting its practical application. To overcome this deficiency, we activated the Olatt of mullite SmMn2O5 through the interface fabrication with spinel Co3O4. The optimized Co3O4/SmMn2O5 catalyst exhibited 90% conversion at 247 °C for the typical automobile exhaust propane combustion, 77 °C lower than the original SmMn2O5. Additionally, Co3O4/SmMn2O5 showed extremely high stability even under harsh operating temperature (e.g., 800 °C). Experimental and theoretical calculation results revealed that the regulated interface of Co3O4/SmMn2O5 facilitated the electrons transfer from SmMn2O5 to Co3O4, contributing to the enhanced propane adsorption and catalytic oxidation activity due to the formation of electrophilic oxygen in SmMn2O5 around the interface. This work can provide a basic understanding of the Olatt activation for developing efficient automobile exhaust combustion catalysts. © 2023 Elsevier B.V.

语种： 英文

作者： Yang, Weiwei;Kim, Mi-Young;Polo-Garzon, Felipe;Gong, Jian;Jiang, Xiao;...

期刊： Chemical Engineering Journal,2023年451:138930 ISSN：1385-8947

通讯作者： Wang, Xiang(xiangwang.chn@gmail.com)

作者机构： [Jiang, Xiao; Wang, Xiang; Yu, Xinbin; Yang, Weiwei; Polo-Garzon, Felipe; Huang, Zhennan; Chi, Miaofang] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA.;[Yang, Weiwei; Guo, Yanbing; Wu, Zili] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Kim, Mi-Young; Gong, Jian] Cummins Inc, Corp Res & Technol, 1900 McKinley Ave, Columbus, IN 47201 USA.

通讯机构： [Xiang Wang; Zili Wu] C;Chemical Science Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, United States

关键词： CH4 oxidation;Commercial Pd/CeO2-ZrO2;Sulfur poisoning;Thermal aging;Three-Way Catalyst

摘要： Thermal aging and sulfur poisoning are major problems influencing the efficiency and lifetime of natural gas three-way catalysts (TWCs) during real-world operation. In the present study, thermal aging and sulfur-induced deactivations on CH4 combustion were investigated over commercial monolithic honeycombs, i.e., Pd/CexZr1-xO2 (CZ)-based TWCs that are thermally aged in the bench (HTA), followed by being operated behind the stoichiometric natural gas engine in high sulfur fuel (HTA + S). Both HTA and HTA + S samples show degraded performance in CH4 combustion relative to the fresh one, which are caused by the reconstruction of Pd species induced by thermal aging and the decreased reducibility of the support. The 18O2 labelling experiments show that in all cases CH4 combustion proceeds via a MvK mechanism in which lattice O (OL) plays a key role. The sulfation aging (HTA + S sample) promotes the activation of CH4 and O2 by forming Pdδ+-(SO42-)δ- and Ce3+-VO couples at the interface as compared to HTA sample. However, such a promotion effect could be compromised by the blocking effect of sulfate on the exchange of OL from the bulk to the surface and across the surface. The fundamental understanding of thermal and S deactivation mechanisms from this study could help to predict a real-world lifetime use curve of natural gas TWCs. © 2022 Elsevier B.V.

语种： 英文

作者： Wang, Peng-Zi;Xiao, Wen-Jing;Chen, Jia-Rong

期刊： ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023年62(21):e202302227- ISSN：1433-7851

通讯作者： Xiao, Wen-Jing(wxiao@mail.ccnu.edu.cn);Chen, Jia-Rong(chenjiarong@mail.ccnu.edu.cn)

作者机构： [Xiao, Wen-Jing; Chen, Jia-Rong; Wang, Peng-Zi] Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Xiao, Wen-Jing; Chen, Jia-Rong] Wuhan Inst Photochem & Technol, 7 North Bingang Rd, Wuhan 430082, Hubei, Peoples R China.

通讯机构： [Prof. Dr. Wen-Jing Xiao; Prof. Dr. Jia-Rong Chen] C;College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei, 430079 China<&wdkj&>Wuhan Institute of Photochemistry and Technology, 7 North Bingang Road, Wuhan, Hubei, 430082 China

关键词： Curtin-Hammett Principle;C−H Carboxylation;Electrochemistry;Radical Anion;SET-Reduction

摘要： Catalytic and switchable C‐H functionalization of N‐heteroarenes under easily tunable conditions is a robust but challenging tool for construction of biologically relevant compounds. Recently, a general electrochemical strategy has been developed for direct C‐H carboxylation of N‐heteroarenes with CO2, and by simply choosing different types of cell setups, carboxylated products are furnished with excellent and tunable site selectivity. This study also paves the way for regulating the reactivity modes in electrochemical synthesis.

语种： 英文

作者： Jiao, Lei;Xu, Weiqing;Wu, Yu;Wang, Hengjia;Hu, Liuyong;...

期刊： Analytical Chemistry,2023年95(1):433-443 ISSN：0003-2700

通讯作者： Zhu, Chengzhou(czzhu@ccnu.edu.cn)

作者机构： [Xu, Weiqing; Zhu, Chengzhou; Wu, Yu; Jiao, Lei; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Bioensing Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Jiao, Lei] Qingdao Univ, Inst Mol Metrol, Coll Chem & Chem Engn, Qingdao 266071, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Hubei Engn Technol Res Ctr Optoelect & New Energy, Sch Mat Sci & Engn, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.

通讯机构： [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, Hubei 430079, P. R. China

语种： 英文

作者： Yang, Heng;Lai, Chunlin;Wu, Mengling;Wang, Shaodan;Xia, Yang;...

期刊： Chemical Engineering Journal,2023年455:140425 ISSN：1385-8947

通讯作者： Wen, Lili(wenlili@mail.ccnu.edu.cn)

作者机构： [Lai, Chunlin; Yang, Heng; Pan, Fangfang; Wu, Mengling; Wen, Lili; Wang, Shaodan] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Xia, Yang] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;[Lv, Kangle] South Cent Minzu Univ, Key Lab Catalysis & Energy Mat Chem, Minist Educ, Wuhan 430074, Peoples R China.;[Wen, Lili] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China.

通讯机构： [Lili Wen] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, PR China<&wdkj&>State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, PR China

关键词： CO2RR;High AQE;MOFs;Open Ni(II) sites;Superior selectivity

摘要： Metal-organic frameworks (MOFs) have aroused ever-growing scientific interest for photocatalytic CO2 reduction reaction (CO2RR). Delicate design and synthesis of MOFs with open metal sites (OMSs) is the key to activate CO2 and even stabilize the reaction intermediates of CO2RR, further determine the superior selectivity. Herein, two amino-functionalized MOFs (Ni-Bpyb and Ni-Bipy) with open Ni(II) sites were constructed from 2′-amino-5′-(4-carboxyphenyl)-[1,1′:3′,1″-terphenyl]-4,4″-dicarboxylic acid (NH2-BTBH3) and different lengths of linear N-donor linkers, 1,4-bis(4-pyridyl) benzene (Bpyb) or 4,4′-bipyridine (Bipy). Under visible-light irradiation, Ni-Bpyb shows more excellent CO yield of 1326.7 μmol·g−1·h−1 with impressive apparent quantum efficiency (AQE, 2.12 %@420 nm) and selectivity (98.80 %). Significantly, this AQE value is at the high end among MOFs-based photocatalysts for CO2RR. The reaction mechanism has been carefully investigated by experimental and theoretical calculations results. Photoelectric experiments demonstrate that Ni-Bpyb shows higher electron–hole separation efficiency compared to Ni-Bipy. Theoretical calculations validate that the open Ni(II) sites of Ni-Bpyb possess lower energy barriers of CO2 adsorption and reducing CO2* to COOH*, as well as better stabilizes COOH* intermediate than those of Ni-Bipy. These merits synergistically contribute to the superior performance and selectivity of Ni-Bpyb. This work might give a guidance for the design of efficient MOFs-based photocatalysts with excellent selectivity for CO2RR. © 2022

语种： 英文

作者： Jia, Shanshan;Zhou, Xin;Yang, Xiaojie;Wang, Xin;Chang, Shao;...

期刊： Analytica Chimica Acta,2023年1265:341267 ISSN：0003-2670

通讯作者： Zhong, HY

作者机构： [Yang, Xiaojie; Zhong, Hongying; Jia, Shanshan] Guangxi Univ, Med Coll, Ctr Instrumental Anal, Nanning 530004, Guangxi, Peoples R China.;[Zhong, Hongying; Liu, Yuqi; Huang, Xingchen; Chang, Shao] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Hubei, Peoples R China.;[Zhong, Hongying; Liu, Yuqi; Huang, Xingchen; Chang, Shao] Guangxi Univ, Coll Life Sci & Technol, Nanning 530004, Guangxi, Peoples R China.;[Wang, Xin] Acad Forens Sci, Shanghai 200063, Peoples R China.;[Zhong, Hongying; Zhong, HY] Guangxi Univ, Ctr Instrumental Anal, Nanning 530004, Guangxi, Peoples R China.

通讯机构： [Zhong, HY ] G;Guangxi Univ, Ctr Instrumental Anal, Nanning 530004, Guangxi, Peoples R China.

关键词： Dynamic features;Handwriting;Laser desorption ionization (LDI);Mass spectrometric imaging;Ultraviolet photodissociation (UVPD)

摘要： Handwriting represents personal education and physical or psychological states. This work describes a chemical imaging technique for document evaluation that combines laser desorption ionization with post ultraviolet photo-induced dissociation (LDI-UVPD) in mass spectrometry. Taken the advantages of chromophores in ink dyes, handwriting papers were subjected to direct laser desorption ionization without additional matrix materials. It is a surface-sensitive analytical method that uses a low intensity pulsed laser at 355 nm to remove chemical components from very outermost surfaces of overlapped handwritings. Meanwhile, the transfer of photoelectrons to those compounds leads to the ionization and the formation of radical anions. The gentle evaporation and ionization property enable the dissection of chronological orders. Paper documents maintain intact without extensive damages after laser irradiation. The evolving plume resulting from the irradiation of the 355 nm laser is fired by the second ultraviolet laser at 266 nm that is in parallel to the sample surface. In contrast to collision activated dissociation in tandem MS/MS, such post ultraviolet photodissociation generates much more different fragment ions through electron-directed specific cleavages of chemical bonds. LDI-UVPD can not only provide graphic representation of chemical components but also reveal hidden dynamic features such as alterations, pressures and aging. © 2023 Elsevier B.V.

语种： 英文

作者： He, Xuan;Tao, Wei;Zhang, Jing-Xuan;Wang, Tao;Shen, Dengke;...

期刊： ACS Materials Letters,2023年5(4):1227-1236 ISSN：2639-4979

通讯作者： Zhang, Zhihan(zhihanzhang@ccnu.edu.cn);Wei, Peifa(pfwei@ahu.edu.cn)

作者机构： [He, Xuan; Tao, Wei; Wei, Peifa; Wang, Tao; Shen, Dengke] Anhui Univ, Inst Phys Sci & Informat Technol, Anhui Graphene Engn Lab, Key Lab Struct & Funct Regulat Hybrid Mat,Minist E, Hefei 230039, Peoples R China.;[Zhang, Jing-Xuan] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China.;[Zhang, Zhihan] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, CCNU uOttawa Joint Res Ctr, Coll Chem,Minist Educ, Wuhan 430079, Hubei, Peoples R China.

通讯机构： [Zhihan Zhang] C;[Peifa Wei] A;Anhui Graphene Engineering Laboratory, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Institutes of Physical Science and Information Technology, Anhui University, Hefei 230039, China<&wdkj&>CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei 430079, China

摘要： To achieve in situ dynamic fluorescence in the solid state and unveil the mechanism remain a formidable challenge. Herein, through synergizing the cavities of macrocycles for dynamic complexing and the channels of frameworks for facile transit, we construct intrinsic channels from an emissive cyclophane and realize precisely tunable emission in the solid state through the sequential guests’ exchange. Specifically, two design criteria involve (1) The twisted cyanostilbene units not only endow the systems with solid-state fluorescence but also tailor the π-π interactions in the complex to generate the desired emission and (2) the large cavity of cyclophane results in the formation of ternary complexes with controllable binding affinity which further assemble into robust channels for the guests’ exchange in the bulky state. This strategy unifies the advantages of both macrocycle and framework in one system, achieving visualization, recyclability, and easy processability simultaneously. The present study paves an easy, efficient, and general platform for constructing dynamic optical materials. © 2023 American Chemical Society

语种： 英文

作者： Ma, Xiaoxie;Huang, Yurou;Chen, Weijie;Liu, Jia;Liu, Sheng Hua;...

期刊： ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023年62(3):e202216109- ISSN：1433-7851

通讯作者： Yin, Jun(yinj@mail.ccnu.edu.cn);Yang, Guang-Fu(gfyang@mail.ccnu.edu.cn)

作者机构： [Huang, Yurou; Yang, Guang-Fu; Liu, Sheng Hua; Chen, Weijie; Yin, Jun; Liu, Jia; Ma, Xiaoxie] Minist Educ, Key Lab Pesticide & Chem Biol, Hubei Int Sci & Technol Cooperat Base Pesticide &, Wuhan, Peoples R China.;[Huang, Yurou; Yang, Guang-Fu; Liu, Sheng Hua; Chen, Weijie; Yin, Jun; Liu, Jia; Ma, Xiaoxie] Int Joint Res Ctr Intelligent Biosensing Technol &, Wuhan, Peoples R China.;[Huang, Yurou; Yang, Guang-Fu; Liu, Sheng Hua; Chen, Weijie; Yin, Jun; Liu, Jia; Ma, Xiaoxie] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.

通讯机构： [Prof. Jun Yin; Prof. Guang-Fu Yang] 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

关键词： Cyanines;Fluorescent Probes;J-Aggregation;Photothermal Therapy;Salt Stress

摘要： The cationic nature of heptamethine cyanines gives them the capacity to form aggregates with salts by electrostatic interactions. In this work, NaCl promoted J-aggregate formation of aza-coating heptamethine cyanines is explored. NaCl can induce the N-benzyloxycarbonyl Cy-CO2Bz to assemble into a J-aggregate having an absorption at 890 nm. Its excellent fluorescence response to NaCl implies that it has great potential for use as a probe for tracing salt stress in plants. Moreover, NaCl also promotes formation of J-aggregates from the N-ethyloxycarbonyl Cy-CO2Et. The aggregate shows an intense absorption at 910 nm compared to the monomer which absorbs at 766 nm. Its J-aggregated form can serve as a photothermal agent. And the photothermal conversion efficiency is increased from 29.37 % to 57.59 %. This effort leads to the development of two applications of new cyanine J-aggregates including one for tracing salt stress of plants and the other for promoting photothermal therapy of tumors.

语种： 英文

作者： Jia, Shanshan;Chang, Shao;Zhang, Lin;Gui, Zhengwei;Liu, Linhui;...

期刊： Analytical Chemistry,2023年95(8):3976-3985 ISSN：0003-2700

通讯作者： Zhong, Hongying(hyzhong@gxu.edu.cn)

作者机构： [Zhong, Hongying; Liu, Linhui; Ma, Zhenglan; Jia, Shanshan] Cent China Normal Univ, Coll Chem, Lab Mass Spectrometry, Key Lab Pesticides & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Zhong, Hongying; Huang, Xingchen; Chang, Shao] Guangxi Univ, Ctr Instrumental Anal, Coll Life Sci & Technol, State Key Lab Conservat & Utilizat Subtrop Agrobio, Nanning 530004, Guangxi, Peoples R China.;[Gui, Zhengwei; Li, Shuyu; Zhang, Lin] Huazhong Univ Sci & Technol, Tongi Med Coll, Wuhan 430030, Hubei, Peoples R China.

通讯机构： [Hongying Zhong] L;Laboratory of Mass Spectrometry, College of Chemistry, Central China Normal University, Key Laboratory of Pesticides and Chemical Biology, Ministry of Education, Wuhan, Hubei 430079, P.R. China<&wdkj&>State Key Laboratory for Conservation and Utilization of Subtropical Agro-Bioresources, College of Life Science and Technology, Guangxi University, Center for Instrumental Analysis of Guangxi University, Nanning, Guangxi 530004, P.R. China

摘要： Lipids represent a large family of compounds with highly diverse structures that are involved in complex biological processes. A photocatalytic technique of on-tissue epoxidation of C=C double bonds has been developed for in situ mass spectrometric identification and spatial imaging of positional isomers of lipids. It is based on the plasmonic hot-electron transfer from irradiated gold nanowires to redox-active organic matrix compounds that undergo bond cleavages and generate hydroxyl radicals in nanoseconds. Intermediate radical anions and negative fragment ions have been unambiguously identified. Under the irradiation of a pulsed laser of the third harmonic of Nd3+:YAG (355 nm), the hydroxyl radical-driven epoxidation of unsaturated lipids with different numbers of C=C bonds can be completed in nanoseconds with high yields of up to 95%. Locations of C=C bonds were recognized with diagnostic fragment ions that were produced by either collision with an inert gas or auto-fragmentation resulting from the impact of energetic hot electrons and vibrational excitation. This technique has been applied to the analysis of breast cancer tissues of mice models without extensive sample processes. It was experimentally demonstrated that C=C bonds may be formed at different positions of not only regular mono- or poly-unsaturated fatty acids but also other odd-numbered long-chain fatty acids. © 2023 American Chemical Society.

语种： 英文

作者： Liao, Minzi;Zhao, Shengxi;Wei, Kai;Sun, Hongwei*;Zhang, Lizhi

期刊： Applied Catalysis B: Environmental,2023年330:122619 ISSN：0926-3373

通讯作者： Sun, Hongwei;Zhang, LZ

作者机构： [Wei, Kai; Zhang, Lizhi; Sun, Hongwei; Liao, Minzi; Zhao, Shengxi; Zhang, LZ] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm & Appl Chem, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.;[Zhang, Lizhi; Sun, Hongwei] Shanghai Jiao Tong Univ, Shanghai Engn Res Ctr Solid Waste Treatment & Reso, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China.

通讯机构： [Sun, HW; Zhang, LZ ] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm & Appl Chem, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.

关键词： Zero-valent iron;Oxalate;Cr(III) complexes;Singlet oxygen;Decomplexation

摘要： Cr(III)-organic complexes removal from wastewater is challenging to decompose the complexes without producing toxic Cr(VI). Herein we demonstrated that oxalated zero-valent iron (Ox-ZVI) could one-step decomplex 95.4% of Cr(III)-EDTA with 94.2% removal of total Cr and 60.5% removal of TOC without generating Cr(VI) at pH 6.0. Ox-ZVI with FeC2O4 shell preferred to adsorb and activate O2 to produce more reactive species than ZVI with iron oxide shell, while the generated 1O2 could selectively break the Cr-O and Cr-N bond to precisely decomplex Cr(III)-EDTA without producing Cr(VI). The released Cr(III) was in-situ precipitated on the surface of ZVI in Cr(OH)3 form. Interestingly, •OH preferred the effective degradation of the released EDTA ligand to the oxidation of the chelated Cr(III) at pH 6.0. This study offers a green and facile method for the Cr(III)-organic complexes treatment, and also sheds light on the importance of reactive species adjustment for the precise pollutant control. © 2023 Elsevier B.V.

语种： 英文