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Boosting CO_(2) electroreduction to formate via bismuth oxide clusters

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Nano Research 2023年第10期16卷 12050-12057页

作者： Xiaole jiang Le Lin Youwen Rong Rongtan Li qike jiang Yaoyue Yang Dunfeng Gao Key Laboratory of Fundamental Chemistry of the State Ethnic Commission School of Chemistry and EnvironmentSouthwest Minzu UniversityChengdu 610041China State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Science Dalian Maritime UniversityDalian 116026China University of Chinese Academy of Sciences Beijing 100049China

Supported metal(oxide)clusters,with both rich surface sites and high atom utilization efficiency,have shown improved activity and selectivity for many catalytic reactions over nanoparticle and single atom ***,the role of cluster catalysts has been rarely reported in CO_(2)electroreduction reaction(CO_(2)RR),which is a promising route for converting CO_(2)to liquid fuels like formic acid with renewable *** we develop a bismuth oxide(BiOn)cluster catalyst for highly efficient CO_(2)RR to *** BiOn cluster catalyst exhibits excellent activity,selectivity,and stability towards formate production,with a formate Faradaic efficiency of over 90%at a current density up to 500 mA·cm^(−2)in an alkaline membrane electrode assembly electrolyzer,corresponding to a mass activity as high as 3,750 A·gBi−*** electrolyzer with the BiOn cluster catalyst delivers a remarkable formate production rate of 0.56 mmol·min−1 at a high single-pass CO_(2)conversion of 44%.Density functional theory calculations indicate that Bi4O_(3)cluster is more favorable for stabilizing the HCOO^(*)intermediate than Bi(001)surface and single site BiC_(4)motif,rationalizing the improved formate production over the BiOn cluster *** work highlights the great importance of cluster catalysts in activity and selectivity control in electrocatalytic CO_(2)conversion.

关键词： CO_(2)electroreduction reaction formate bismuth oxide cluster catalyst membrane electrode assembly

Pd single-atom catalysts derived from strong metal-support interaction for selective hydrogenation of acetylene

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Nano Research 2022年第12期15卷 10037-10043页

作者： Yalin Guo Yangyang Li Xiaorui Du Lin Li qike jiang Botao Qiao CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of Chinese Academy of Sciences Beijing100049China Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou510640China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China

Selective hydrogenation of acetylene in excess ethylene is an important reaction in both fundamental study and practical ***-based catalysts with high intrinsic activity are commonly employed,but usually suffer from low *** single-atom catalysts(SACs)usually exhibit outstanding ethylene selectivity due to the weakπ-bonding ethylene ***,the preparation of high-loading and stable Pd SACs is still confronted with a great *** this work,we report a simple strategy to fabricate Pd SACs by means of reducing conventional supported Pd catalysts at suitable temperatures to selectively encapsulate the co-existed Pd nanoparticles(NPs)/*** is based on our new finding that single atoms only manifest strong metal-support interaction(SMSI)at higher reduction temperature than that of NPs/*** derived Pd SACs(Pd1/CeO2 and Pd1/a-Fe2O3)were applied to acetylene selective hydrogenation,exhibiting much improved ethylene selectivity and high *** work offers a promising way to develop stable Pd SACs easily.

关键词： selective hydrogenation of acetylene Pd single-atom catalysts(SACs) weakπ-bonding ethylene adsorption strong metal-support interaction(SMSI)

Synthesis and characterization of anatase TiO_2 nanosheet arrays on FTO substrate

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Journal of Energy Chemistry 2015年第5期24卷 626-631页

作者： Dong Zhong qike jiang Baokun Huang Wen-Hua Zhang Can Li State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian National Laboratory for Clean Energy

We have exploited a green approach to prepare layered titanate Na2_xHxTi2Os-H20 nanosheet arrays on FFO substrate by hydrothermal hydrolysis of titanium（IV） isopropoxide （TRIP） with aids of Na2EDTA and TEOA as co-coordination agents, which were then treated by HNO3 to replace Na＋ by H＋, followed by a calcination at 450℃ to topotactically transform into anatase TiO2 nanosheet arrays. SEM, TEM, XRD, and Raman spectroscopy have been employed to characterize the nanosheet films. The TiO2 nanosheet arrays were further applied as electron transport materials of CH3NH3PbI3 perovskite solar cells, achieving power conversion efficiency of 6.99%.

关键词： Anatase TiO2 Nanosheet Hydrothermal synthesis Perovskite solar cells

Selective and stable Au-Cu bimetallic catalyst for CO-PROX

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Nano Research 2023年第7期16卷 9031-9038页

作者： Feng Hong Guanjian Cheng Weihao Hu Shengyang Wang qike jiang Junhong Fu Botao Qiao Jiahui Huang Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of Energy Soochow Institute for Energy and Materials Innovations(SIEMIS)Soochow UniversitySuzhou 215006China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China School of Chemistry and Chemical Engineering Yulin UniversityYulin 719000China University of Chinese Academy of Sciences Beijing 100049China

Gold-based catalysts are promising in CO preferential oxidation(CO-PROX)reaction in H_(2)-rich stream on account of their high intrinsic activity for CO elimination even at ambient ***,the decrease of CO conversion at elevated temperature due to the competition of H_(2)oxidation,together with the low stability of gold nanoparticles,has posed a dear ***,we report that Au-Cu bimetallic catalyst prepared by galvanic replacement method shows a wide temperature window for CO total conversion(30-100℃)and very good catalyst stability without deactivation in a 200-h *** characterizations combined with density functional theory(DFT)calculation reveal that the synergistic effect of Au-Cu,the electron transfer from Au to Cu,leads to not only strengthened chemisorption of CO but also weakened dissociation of H_(2),both of which are helpful in inhibiting the competition of H_(2)oxidation thus widening the temperature window for CO total conversion.

关键词： gold catalysis CO preferential oxidation(CO-PROX) electronic interaction galvanic replacement

Wavy PtCu alloy nanowire networks with abundant surface defects enhanced oxygen reduction reaction

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Nano Research 2019年第11期12卷 2766-2773页

作者： Dahui Fang Lei Wan qike jiang Hongjie Zhang Xuejun Tang Xiaoping Qin Zhigang Shao Zidong Wei Fuel Cell Systerm and Engineering Laboratory Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Bejing 100049China The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversitBeijing 100084China Advanced Electrorn Microscopy Research Group Dalian Inrstitute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of Chemistry and Chemical Engineering Chongqing UniversityChongqing 400044China

Bimetalic platinum-copper(Pt-Cu)alloy nanowires have emerged as a novel class of fuel cell electrocatalysts for oxygen reduction reaction(ORR)due to their intrinsic high catalytic activity and durability,but preparing such electrocatalysts with clean surface via facile method is still a ***,PtCu alloy with nanowire networks(NWNs)structure is obtained by a simple modified polyol method accompanied with a salt-mediated self-assembly process in a water/ethylene glycol(EG)mixing *** formation mechanism of PtCu NWNs including the morphological evolution and the relevant experimental parameters has been investigated *** propose that a micro-interface in H2O-EG media formed with the assistance of disodium dihydrogen pyrophosphate(Na2H2P2O7)and its unique nature of coordinating with Pt^2+ or Cu^2+ play critical roles in the formation of *** tested as ORR catalyst,the PtCuNWNs/C exhibits much higher activity and durability than that of PtNWNs/C and commercial PtC,even exceeding the target of DOE in *** excellent performance of PtCuNWNs/C could be attributed to the unique structure of NWNs with 2.4 nm ultrathin wavy nanowires and plentiful surface defects and the modified electronic effect caused by alloying with Cu atoms.

关键词： PtCu nanoalloy nanowire networks surface defect self-assembly,oxygen reduction reaction

High performance perovskite solar cells using TiO2 nanospindles as ultrathin mesoporous layer

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Journal of Energy Chemistry 2018年第4期27卷 951-956页

作者： Yinhua Lv Bing Cai Yihui Wu Shubo Wang qike jiang Qingshan Ma Jingyue(Jimmy)Liu Wen-Hua Zhang Dalian National Laboratory for Clean Energy.Dalian Institute of Chemical Physics Chinese Academy of Sciences.Dalian 116023LiaoningChina University of Chinese Academy of Sciences No.19(A)Yuquan Road.Shijingshan DistrictBeijing 100049.China Sichuan Research Center of New Materials Institute of Chemical MaterialsChina Academy of Engineering PhysicsChengdu 610200.Sichuan.China jiangsu Collaborative Innovation Center of Photovoltuic Science an Engineering.Changzhou University Changzhou 213164JiangsuChina Department of Physics Arizona State UniversityTempeArizona 85287.USA

Single crystal anatase TiO2 nanospindles （NSs） with highly exposed {101} facets were synthesized and employed as electron transport materials （ETMs） in perovskite solar cells （PSCs）. Time-resolved photoluminescence （TRPL） spectra revealed that the TiO2 NSs are more effective than TiO2 nanoparticles in accepting electrons from perovskite. Moreover. the TiO2 nanospindles further endowed the PSCs with good reproducibility and suppressed hysteresis. The best device with TiO2 NSs as ETMs yielded power conversion efficiency （PCE） of 19.6%, demonstrating that the home-made TiO2 NSs is a good ETM for PSCs.

关键词： Electron transport material Perovskite solar cell TiO2 nanospindles Ultrathin mesoporous layer

Strong metal‐support interaction boosting the catalytic activity of Au/TiO_(2) in chemoselective hydrogenation

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Chinese Journal of Catalysis 2021年第9期42卷 1530-1537页

作者： Feng Hong Shengyang Wang Junying Zhang Junhong Fu qike jiang Keju Sun Jiahui Huang Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Key Laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004HebeiChina

Gold catalysts have been reported as highly effective catalysts in various oxidation ***,for chemoselective hydrogenation reactions,gold‐based catalysts normally show much lowercatalytic activity than platinum group metals,even though their selectivities are ***,wereport that the chemoselective hydrogenation activity of 3‐nitrostyrene to 3‐vinylaniline overAu/TiO_(2)can be enhanced up to 3.3 times through the hydrogen reduction *** is revealedthat strong metal‐support interaction,between gold nanoparticles(NPs)and TiO_(2)support,is introducedthrough hydrogen reduction,resulting in partial dispersion of reduced TiOx on the Au *** partially covered Au not only increases the perimeter of the interface between the gold NPs andthe support,but also benefits H_(2)*** kinetic analysis and H_(2)‐D2 exchange reactionshow that H_(2)activation is the critical step in the hydrogenation of 3‐nitrostyrene to 3‐*** functional theory calculations verify that hydrogen dissociation and hydrogen transfer arefavored at the interface of gold NPs and TiO_(2)over the hydrogen‐reduced Au/TiO_(2).This study providesinsights for fabricating highly active gold‐based catalysts for chemoselective hydrogenationreactions.

关键词： Gold catalysis Strong metal support interaction Interface 3‐Nitrostyrene chemoselective hydrogenation Boosting activity

Fe atoms anchored on defective nitrogen doped hollow carbon spheres as efficient electrocatalysts for oxygen reduction reaction

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Nano Research 2021年第4期14卷 1069-1077页

作者： Panpan Su Wenjuan Huang jiangwei Zhang Utsab Guharoy Qinggang Du Qiao Sun qike jiang Yi Cheng Jie Yang Xiaoli Zhang Yongsheng Liu San Ping jiang Jian Liu College of Mathematics and Physics Shanghai University of Electric PowerShanghai 200090China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of Radiation Medicine and Protection Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSchool for Radiological and Interdisciplinary SciencesSoochow UniversitySuzhou 215123China Division of Energy Research Resourcesy Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China Department of Environmental Engineering School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWA 6102Australia State Centre for International Cooperation on Designer Low-Carbon&Environmental Materials School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China DICP-Surrey Joint Centre for Future Materials Department of Chemical and Process EngineeringUniversity of SurreyGuildfordSurreyU K

Defective electrocatalysts,especially for intrinsic defective carbon,have aroused a wide concern owing to high spin and charge ***,the designated nitrogen species favorable for creating defects by the removal of nitrogen,and the influence of defects for the coordination structure of active site and oxygen reduction reaction(ORR)activity have not been ***,we designed and synthesized a pair of electrocatalysts,denoted as Fe-N/C and Fe-ND/C for coordination sites of atomic iron-nitrogen and iron-nitrogen/defect configuration embedded in hollow carbon spheres,respectively,through direct pyrolysis of their corresponding hollow carbon spheres adsorbed with Fe(acac)*** nitrogen defects were fabricated via the evaporation of pyrrolic-N on nitrogen doped hollow carbon *** of comparative experiments between Fe-N/C and Fe-ND/C reveal that Fe-ND/C shows superior ORR activity with an onset potential of 30 mV higher than that of Fe-N/***-ND sites are more favorable for the enhancement of ORR *** functional theory(DFT)calculation demonstrates that Fe-ND/C with proposed coordination structure of FeN_(4-x)(0

关键词： atom ic iron nitrogen defect coordination environment hollow carbon spheres oxygen reduction reaction

Reaction kinetics and phase behavior in the chemoselective hydrogenation of 3‐nitrostyrene over Co‐N‐C single‐atom catalyst in compressed CO_(2)

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Chinese Journal of Catalysis 2021年第9期42卷 1617-1624页

作者： Dan Zhou Leilei Zhang Wengang Liu Gang Xu Ji Yang qike jiang Aiqin Wang Jianzhong Yin School of Chemical Engineering State Key Laboratory of Fine ChemicalsDalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Single‐atom catalysts(SACs)have demonstrated excellent performances in chemoselective hydrogenation ***,the employment of precious metals and/or organic solvents compromises their ***,we for the first time report the chemoselective hydrogenation of 3‐nitrostyrene over noble‐metal‐free Co‐N‐C SAC in green solvent—compressed *** interesting inverted V‐curve relation is observed between the catalytic activity and CO2 pressure,where the conversion of 3‐nitrostyrene reaches the maximum of 100%at 5.0 MPa CO2(total pressure of 8.1 MPa).Meanwhile,the selectivities to 3‐vinylaniline at all pressures remain high(>99%).Phase behavior studies reveal that,in sharp contrast with the single phase which is formed at total pressure above 10.8 MPa,bi‐phase composed of CO2/H_(2)gas‐rich phase and CO2‐expanded substrate liquid phase forms at total pressure of 8.1 MPa,which dramatically changes the reaction kinetics of the catalytic *** reaction order with respect to H_(2)pressure decreases from~0.5 to zero at total pressure of 8.1 MPa,suggesting the dissolved CO2 in 3‐nitrostyrene greatly promotes the dissolution of H_(2)in the substrate,which is responsible for the high catalytic activity at the peak of the inverted V‐curve.

关键词： Single‐atom catalyst Co‐N‐C CO2 Phase behavior Chemoselective hydrogenation 3‐Nitrostyrene