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The configuration of Au^(δ+)-ZrO_(2)^(δ−)species induced activation enhances electrocatalytic CO_(2)to formate conversion

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Nano Research 2024年第7期17卷 6006-6015页

作者： Yongjian Jia Yadi Zhang Mengque Lin Yangyang Cheng Yanjie Xu National Engineering Research Center for Technology and Equipment of Environmental Deposition Lanzhou Jiaotong UniversityLanzhou 730070China Key Lab of Opt-Electronic Technology and Intelligent Control of Ministry of Education Lanzhou Jiaotong UniversityLanzhou 730070China School of Environmental Engineering and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471023China

Electrochemical CO_(2)conversion into value-added chemicals is a promising technology to solve the greenhouse effect and recycle chemical ***,the electrochemical CO_(2)reduction reaction(e-CO_(2)RR)is seriously compromised by weak CO_(2)adsorption and a rough CO_(2)activation process based on the chemical inertness of the CO_(2)molecule and the formed fragile metal–C/O *** this paper,we designed and fabricated Au particles embedded in ZrO_(2).The configuration of Au particles being of positive charge and ZrO_(2)with negative charge is induced and generated by metal–support interactions(MSIs).As a result,Au/ZrO_(2)@C presents a big difference in the CO_(2)conversion compared with the known work,affording a formate yield of 112.5μmol·cm^(−2)·h^(−1)at−1.1 V *** hydrogen electrode(RHE),and a max formate Faradaic efficiency of up to 94.1%at−0.9 V *** superior performance was attributed to the activated Au–ZrO_(2)interface to form the Au^(δ+)*** insitu Fourier transform infrared(FTIR)spectroscopy and theoretical calculations show that the MSIs configuration can be inclined to the*OCO intermediate generation on Au^(δ+)species activating CO_(2)molecules and then accelerate the formation of the*OCHO intermediate in e-CO_(2)RR,thereby favoring the CO_(2)conversion to formate.

关键词： electrochemical CO_(2)reduction reaction(e-CO_(2)RR) Au_(δ+)species formic acid *OCHO intermediate metal-support interactions

Oxygen reduction electrocatalysis:From conventional to single-atomic platinum-based catalysts for proton exchange membrane fuel cells

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Frontiers in Energy 2024年第2期18卷 206-222页

作者： Cheng YUAN Shiming ZHANG Jiujun ZHANG Institute for Sustainable Energy/College of Sciences Shanghai UniversityShanghai 200444China

Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading *** on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts,Pt single-atom catalysts(Pt SACs)as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this *** design thoughts and synthesis of various isolated,alloyed,and nanoparticlecontained Pt SACs are *** single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the *** advance further research and development of Pt SACs for viable implementation in PEMFCs,various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis Pt singleatom catalysts conventional Pt-based catalysts design thoughts and synthesis metal-support interactions

Investigating the impact of dynamic structural changes of Au/rutile catalysts on the catalytic activity of CO oxidation

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Carbon Energy 2024年第4期6卷 222-232页

作者： Xiaochun Hu Qianwenhao Fan Mingwu Tan Yuqing Luo Xianyue Wu Manoel Y.Manuputty Jie Ding Tej S.Choksi Markus Kraft Rong Xu Zhiqiang Sun Wen Liu School of Energy Science and Engineering Central South UniversityChangshaChina School of Chemistry Chemical Engineering and BiotechnologyNanyang Technological UniversitySingaporeSingapore Cambridge Centre for Advanced Research and Education SingaporeSingapore Institute of Sustainability for Chemicals Energy and EnvironmentJurong IslandSingapore College of Chemistry and Chemical Engineering Central South UniversityChangshaChina Department of Chemical Engineering and Biotechnology University of CambridgeCambridgeUK

The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal *** metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active ***,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe *** analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) *** the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains *** functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation.

关键词： CO oxidation electronic metal-support interactions flame‐synthesis metal-support interactions oxygen vacancy strong metal-support interaction

The modification of titanium in mesoporous silica for Co-based Fischer–Tropsch catalysts

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Frontiers of Chemical Science and Engineering 2022年第8期16卷 1224-1236页

作者： Xin Li Meng Su Yao Chen Mehar UNisa Ning Zhao Xiangning Jiang Zhenhua Li Key Lab for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin UniversityTianjin 300072China Research Institute of Petroleum Processing SINOPECBeijing 100083China

Ordered SBA-15 mesoporous silica with incorporated titanium was successfully synthesized via a onepot hydrothermal crystallization *** characterization including powder X-ray diffraction,Brunauer–Emmett–Teller,transmission electron microscope,temperatureprogrammed reduction,temperature-programmed desorption,Fourier transform infrared and ultraviolet-visible-near infrared spectrometer was performed to explore the physical and chemical structures of both the supports and the *** results showed that titanium was successfully incorporated into the mesoporous silica framework with a limited amount of titanium(Si/Ti>20),and the mesoporous structure was ***,the increased titanium content inevitably resulted in the formation of anatase TiO2 particles on the support *** increased incorporated titanium strengthened the interactions between cobalt species and supports,which was favorable for the cobalt species dispersion,despite the limited cobalt oxide *** enhanced metalsupport interactions were beneficial for the CO/H2 ratio at the active cobalt sites,which facilitated the formation of more C5+*** study provides a promising method for support modification with incorporatedheteroatoms for the rational development of Fischer–Tropsch catalysts.

关键词： Fischer–Tropsch synthesis titanium incorporation mesoporous silica metal-support interactions C5+selectivity

In situ confined vertical growth of Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)nanoarrays on rGO for an efficient oxygen evolution reaction

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Nano Materials Science 2023年第4期5卷 351-360页

作者： Yang Mu Xiaoyu Pei Yunfeng Zhao Xueying Dong Zongkui Kou Miao Cui Changgong Meng Yifu Zhang State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian116024China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China

Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the *** advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER *** to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@*** CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)*** achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their *** vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron *** advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.

关键词： Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)@rGO Vertical grown nanoarrays Geometric and electronic structure regulation metal-support interactions Oxygen evolution reaction

Strong High Entropy Alloy-support Interaction Enables Efficient Electrocatalytic Water Splitting at High Current Density

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Chinese Journal of Structural Chemistry 2022年第8期41卷 3-11页

作者： Hongdong Li Yue Pan Jianping Lai Lei Wang Shouhua Feng Key Laboratory of Eco-chemical Engineering Taishan Scholar Advantage and Characteristic Discipline Team of Eco-chemical Process and TechnologyCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

In electrocatalysis, the stability issue between catalyst and support still needs great attention. Here, a series of highentropy alloy nanoparticles(HEA-NPs) embedded in carbon cloth(CC) were synthesized by using the scalable strategy-microwave heating. Among them, PtRhCoNiCu/CC exhibits outstanding hydrogen evolution reaction(HER) activity(19 and 170 mV overpotential at 10 and 1000 mA cm^(-2)) and stability(150 h), outperforming other recently reported HEAs catalysts. IrRuCoNiCu/CC displays superior oxygen evolution reaction(OER) activity(166 and 354 mV overpotential at 10 and 1000 m A cm^(-2)) and stability(150 h), and shows a lower overpotential than recently reported HEA catalysts. In water splitting, IrRuCoNiCu/CC(+)//Pt Rh Co Ni Cu/CC(-) electrolyzer achieves 500 m A cm^(-2)(1000 m A cm^(-2)) high current density at 1.76 V(1.88 V) and exhibits excellent stability, which is one of the best catalysts currently. Therefore, the novel supported HEA catalyst with high stability is expected to be a promising candidate material for industrialized water splitting.

关键词： high entropy alloy metal-support interactions microwave heating water splitting activity and durability

Recent Advances in the Catalytic Upgrading of Biomass Platform Chemicals Via Hydrotalcite-Derived metal Catalysts

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Transactions of Tianjin University 2022年第2期28卷 89-111页

作者： Zhe-Hui Zhang Zhuohua Sun Tong-Qi Yuan Beijing Key Laboratory of Lignocellulosic Chemistry Beijing Forestry UniversityBeijing 100083China

With the world’s fossil fuels being finite in nature,an increasing interest focuses on the application of alternative renewable resources such as ***-derived platform chemicals with abundant functional groups have the potential to replace bulk chemicals for the production of value-added chemicals,fuels,and *** upgrading of these platform chemicals relies on the development of efficient catalytic ***,with its wide compositional variety,tuneable anion-exchange capacity,and controlled acidity/basicity sites demonstrates great potential in the catalytic upgrading of biomass and the derived platform *** past decade has witnessed the emergence of research achievements on the development of efficient and robust hydrotalcite-derived metal catalysts and their applications in the upgrading of biomass or the derived platform *** this review,we aim to summarize the recent advances on the catalytic upgrading of biomass-derived platform chemicals(e.g.,furfural,5-hydroxymethylfurfural,levulinic acid,and glycerol)via hydrotalcitederived metal *** also observed that the crucial role of using hydrotalcite-derived catalysts relies on their strong metal–support *** a result,a section focusing on the discussion of the metal–support interactions of hydrotalcitederived catalysts was provided.

关键词： Hydrotalcite Biomass Catalysis metal-support interactions

Ultrafine Pt nanoparticles supported on double-shelled C/TiO2 hollow spheres material as highly efficient methanol oxidation catalysts

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Journal of Energy Chemistry 2020年第10期29卷 275-282页

作者： Xiaoyu Yue Yuguang Pu Wen Zhang Ting Zhang Wei Gao Department of Chemical and Materials Engineering the University of AucklandPrivate Bag 92019Auckland 1142New Zealand

Catalyst support is extremely important for future fuel cell *** this work,we developed doubleshelled C/TiO2(DSCT)hollow spheres as an excellent catalyst support via a template-directed *** combination of hollow structure,TiO2 shell and carbon layer results in excellent electron conductivity,electrocatalytic activity,and chemical *** uniformed DSCT hollow spheres are used as catalyst support to synthesize Pt/DSCT hollow spheres *** resulting Pt/DSCT hollow spheres exhibited high catalytic performance with a current density of 462 mA mg^-1 for methanol oxidation reaction,which is 2.52 times higher than that of the commercial Pt/***,the increased tolerance to carbonaceous poisoning with a higher If/Ibratio and a better long-term stability in acid media suggests that the DSCT hollow sphere is a promising C/TiO2-based catalyst support for direct methanol fuel cells applications.

关键词： Catalyst support C/TiO2 hollow sphere metal-support interactions Methanol oxidation reaction

Promoting NO_(x)reduction via in situ activation of perovskite supported Pd catalysts under alternating lean-burn/fuel-rich operating atmospheres

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Chinese Journal of Catalysis 2021年第5期42卷 795-807页

作者： Dongyue Zhao Yuexi Yang Zhongnan Gao Mengxin Yin Ye Tian Jing Zhang Zheng Jiang Xiaobo Yu Xingang Li Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin Key Laboratory of Applied Catalysis Science and TechnologySchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China College of Materials Science and Engineering Jilin Institute of Chemical TechnologyJilin 132022JilinChina

Herein,we report the excellent De-NO_(x)performance of La0.7Sr0.3MnO3(LSM)perovskite-supported Pd catalysts(Pd-LSM)in alternating lean-burn/fuel-rich atmospheres using C3H6 as reductant and describe the in situ activation of the Pd catalysts via metal-support interaction(MSI)*** NO_(x)reduction conversion of the Pd-LSM catalyst increased significantly from 56.1%to 90.1%and the production of N2O was *** results demonstrated that this behavior was mainly attributed to the in situ transformation of Pd2+into Pd0 during the *** generated Pd0 species could readily activate the C3H6 reductant and achieve an eight-fold higher turnover frequency than Pd2+for the reduction of NO_(x).Moreover,excessive MSIs inhibited the in situ generation of Pd0,and thereby,lowered the De-NO_(x)activity of the catalyst even at high Pd *** addition,the Pd-LSM catalysts exhibited much higher S tolerance than conventional Al_(2)O_(3)-supported *** study provides a new approach for analyzing and designing highly active metal catalysts operated under dynamic alternating oxidizing/reducing atmospheric conditions.

关键词： Lean-burn NO_(x)reduction metal-support interactions In situ activation Pd