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A hybrid artificial photosynthesis system with molecular catalysts covalently linked onto TiO2 as electron relay for efficient photocatalytic hydrogen evolution

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Journal of Materials Science & Technology 2020年第15期47卷 147-152页

作者： Jie Zhang Gehong Zhang Jing Zhang School of Civil and Architecture Engineering Xi'an Technological UniversityXi'an710021China

Efficient charge carrier transfer from light harvesters to catalysts greatly determines the photocatalytic activity in an artificial photosynthesis(AP) system for solar hydrogen *** this study,an AP system composed of xanthene dye as light harvester and cobaloxime molecular complex as catalyst,with TiO2 as electron relay,was designed for photocatalytic hydrogen evolution under visible light(λ>420 nm).It was demonstrated that with cobaloxime molecule covalently linked onto the TiO2 electron relay,the resulting hybrid AP system exhibited much increased photocatalytic activity as compared to that without *** greatly increased photocatalytic activity should be due to the efficient electron transfer from xanthene dye as light harvester and cobaloxime molecular complex as catalyst,shuttled by the TiO2 electron relay,for the following water reduction *** present study demonstrates a facile and feasible strategy to guide the design of high performance AP systems through the electron relay shuttled and promoted cha rge transfer process.

关键词： Artificial photosynthesis molecular catalysts Electron relay Photocatalytic hydrogen evolution

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Smart tailoring of molecular catalysts:Mounting approach to oxygen reduction reaction

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Journal of Materials Science & Technology 2024年第1期168卷 169-184页

作者： Anuj Kumar Mohd Ubaidullah Guoxin Zhang Jasvinder Kaur Saira Ajmal Mudassir Hasan Krishna Kumar Yadav Hafiz M.Adeel Sharif Ram K.Gupta Ghulam Yasin Nano-Technology Research Laboratory Department of ChemistryGLA UniversityMathuraUttar Pradesh 281406India Department of Chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia Department of Electrical Engineering and Automation Shandong University of Science and TechnologyQingdaoShandong 266590China Institute for Advanced Study Shenzhen UniversityShenzhenGuangdong 518060China Department of Chemistry Kansas Polymer Research CenterPittsburg State UniversityPittsburgKS 66762United States Faculty of Science and Technology Madhyanchal Professional UniversityRatibadBhopal 462044India Environmental and Atmospheric Sciences Research Group Scientific Research CenterAl-Ayen UniversityThi-QarNasiriyah 64001Iraq Department of Chemical Engineering King Khalid University Saudi Arabia Department of Chemistry School of SciencesIFTM UniversityMoradabadUttar Pradesh 244102India Research Center for Eco-Environmental Engineering Dongguan University of TechnologyDongguan 523808China School of Environment and Civil Engineering Dongguan University of TechnologyDongguanGuangdong 523808China

Efficient electrocatalytic rupture of energy-rich molecules(H_(2)and O_(2))is a green approach for gener-ating clean energy for modern *** this context,porphyry-type molecular electrocatalysts act intelligently toward oxygen reduction reaction(ORR),a fundamental process in fuel cells,due to their redox-rich chemistry,which involves core metal ions and macrocyclic *** concerned scientific community has tried many times to correlate the ORR intermediates with their formation kinetics and simplify the associated multi H+/e-stages during the ORR process,constructing several volcano plots be-tween catalytic Tafel data,turnover frequencies,and overpotentials for many *** the fact that many review articles on molecular electrocatalysts for ORR have been published,understanding the strategic implications and molecular catalyst intelligence towards homogenous ORR has been poorly *** review examined the relationships between volcano plots of current *** parameters and the Sabatier principle in order to explain the intelligence of molecular electrocatalysts and approaches for their creation,as well as the difficulties and potential prospects of molecular *** facts distinguish this review from previously published articles and will pique the scien-tific community’s interest in avoiding trial-and-error procedures for catalyst creation while also allowing for more exact evaluations of the molecular catalyst’s performance.

关键词： Electrocatalysis molecular catalysts Oxygen reduction reaction Sabatier principle

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Tuning electronic properties of cobalt phthalocyanines for oxygen reduction and evolution reactions

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Science China Chemistry 2024年第1期67卷 398-407页

作者： Jianlin Jiang Zhen Liu Shuaijun Pan Xinnian Xia Bing Qin Yang Hu Xuxu Wang Jiamin Lan Yu Gu Encai Ou Weijian Xu Joseph J.Richardson Rui Guo SINOPEC Research Institute of Petroleum Processing Co. Ltd.Beijing 100083China College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China College of Chemistry and Materials Science Hunan Agricultural UniversityChangsha 410128China Department of Chemical Engineering The University of MelbourneParkville 3010Australia College of Environmental Science and Engineering Hunan UniversityChangsha 410082China School of Engineering RMIT UniversityMelbourneVictoria 3001Australia

Metal–phthalocyanines are a class of catalytically active materials promising in energy conversion and storage fields(e.g.,electrocatalysis).However,understanding and controlling the electrochemical properties in metal-phthalocyanine systems is ***,we elucidate the electrocatalytic origins of a series of cobalt-phthalocyanine molecular catalysts and finetune their electronic properties at the atomic level,both experimentally and *** interactions between the cobalt center and the local coordination environment are regulated by introducing either electron-donating or electron-withdrawing groups on the phthalocyanine ligand,and the spin-orbit splitting of cobalt is increased by~0.15 eV compared with the nonsubstituted ***,the aminated cobalt phthalocyanine-based electrocatalysts exhibit low free energies in the ratedetermining steps of the oxygen reduction(-1.68 eV)and oxygen evolution reactions(0.37 eV).This contributes to the high electrocatalytic activity(e.g.,a halfwave potential of 0.84 V and an overpotential of 0.30 V at 10 mAcm^(-2)),featuring a high selectivity of a four-electron pathway(i.e.,a negligible by-product of hydrogen peroxide).These catalysts also exhibit exceptional kinetic current density(Tafel slope of 100 mV dec^(-1))in oxygen reduction reactions,in addition to a superior power density(158 mWcm^(-2))and a high cycling stability(>1,300 cycles)in Zn-air batteries,outperforming the commercial Pt/C and/or RuO2counterparts.

关键词： interfacial wettability molecular catalysts carbon nanotubes density functional theory electrochemistry

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A perspective on the electrocatalytic conversion of carbon dioxide to methanol with metallomacrocyclic catalysts

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Journal of Energy Chemistry 2022年第1期31卷 263-275,I0008页

作者： Xinyan Liu Bo-Quan Li Bing Ni Lei Wang Hong-Jie Peng Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Physical Chemistry Department of ChemistryUniversity of KonstanzUniversitatsstrasse 10D-78457 KonstanzGermany Department of Chemical and Biomolecular Engineering National University of Singapore.Singapore 117585Singapore

Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy *** is an ideal energy carrier as alternative fuels and one of the most important commodity ***,methanol is currently mainly produced from fossil-based syngas,the production of which yields tremendous carb on emission *** CO_(2)R towards metha nol poses great potential to shift the paradigm of methanol *** this perspective,we focus our discussions on producing methanol from electrochemical CO_(2)R,using metallomacrocyclic molecules as the model *** discuss the motivation of having methanol as the sole CO_(2)R product,the documented application of metallomacrocyclic catalysts for CO_(2)R,and recent advance in catalyzing CO_(2) to methanol with cobalt phthalocyanine-based *** attempt to understand the key factors in determining the activity,selectivity,and stability of electrocatalytic CO_(2)-to-methanol conversion,and to draw mechanistic insights from existing ***,we identify the challenges hindering methanol electrosynthesis directly from CO_(2) and some intriguing directions worthy of further investigation and exploration.

关键词： Carbon dioxide reduction Methanol Electrocatalysis molecular catalysts Single atom catalysts Heterogenization

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