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Tailoring local structures of atomically dispersed copper sites for highly selective CO2 electroreduction

Carbon Energy 2024年第4期6卷 79-90页

作者： Kyung‐Jong Noh Byoung Joon Park Ying Wang Yejung Choi Sang‐Hoon You Yong‐Tae Kim Kug‐Seung Lee Jeong Woo Han department of Chemical Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbukRepublic of Korea department of Materials Science and Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbukRepublic of Korea Pohang Accelerator Laboratory(PAL) Beamline DivisionPohangGyeongbukRepublic of Korea

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm–2 at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.

关键词： atomic local structure density functional theory electrochemical CO_(2)reduction metal nitrogen‐doped carbon single‐atom catalyst

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Tuning electronic structure of RuO_(2)by single atom Zn and oxygen vacancies to boost oxygen evolution reaction in acidic medium

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Journal of Energy Chemistry 2024年第1期88卷 94-102,I0003页

作者： Qing Qin Tiantian Wang Zijian Li Guolin Zhang Haeseong Jang Liqiang Hou Yu Wang Min Gyu Kim Shangguo Liu Xien Liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina department of Chemistry City University of Hong KongHong Kong 999077China department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-do 17546SeoulRepublic of Korea beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang 37673Gyeongsangbuk-doRepublic of Korea

The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.

关键词： Electrocatalyst Acidic oxygen evolution reaction Electronic structure engineering Durability Reaction barrier

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Electron-deficient ZnO induced by heterointerface engineering as the dominant active component to boost CO_(2)-to-formate conversion

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Carbon Energy 2024年第5期6卷 127-136页

作者： Qing Qin Zijian Li Yingzheng Zhang Haeseong Jang Li Zhai Liqiang Hou Xiaoqian Wei Zhe Wang Min Gyu Kim Shangguo Liu Xien Liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdaoChina department of Chemistry City University of Hong KongHong Kong SARChina department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-doRepublic of Korea beamline Research Division Pohang Accelerator Laboratory(PAL)PohangRepublic of Korea

Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.

关键词： charge redistribution CO_(2)reduction reaction electrocatalyst heterointerfaces selectivity

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Surface-modified Ag@Ru-P25 for photocatalytic CO_(2) conversion with high selectivity over CH_(4) formation at the solid–gas interface

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Carbon Energy 2024年第1期6卷 182-196页

作者： Chaitanya B.Hiragond Sohag Biswas Niket SPowar Junho Lee Eunhee Gong Hwapyong Kim Hong Soo Kim Jin-Woo Jung Chang-Hee Cho Bryan M.Wong Su-Il In department of Energy Science&Engineering Daegu Gyeongbuk Institute of Science and Technology(DGIST)DaeguRepublic of Korea department of Chemical&Environmental Engineering Materials Science&Engineering ProgramDepartment of ChemistryDepartment of Physics&AstronomyUniversity of California-RiversideRiversideCaliforniaUSA department of Physics and Chemistry Daegu Gyeongbuk Institute of Science and Technology(DGIST)DaeguRepublic of Korea NiceScience Corporation DaeguRepublic of Korea

Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar fuels.A surface-modified Ag@Ru-P25 photocatalyst with H_(2)O_(2) treatment was designed in this study to convert CO_(2) and H_(2)O vapor into highly selective CH4.Ru doping followed by Ag nanoparticles(NPs)cocatalyst deposition on P25(TiO_(2))enhances visible light absorption and charge separation,whereas H_(2)O_(2) treatment modifies the surface of the photocatalyst with hydroxyl(–OH)groups and promotes CO_(2) adsorption.High-resonance transmission electron microscopy,X-ray photoelectron spectroscopy,X-ray absorption near-edge structure,and extended X-ray absorption fine structure techniques were used to analyze the surface and chemical composition of the photocatalyst,while thermogravimetric analysis,CO_(2) adsorption isotherm,and temperature programmed desorption study were performed to examine the significance of H_(2)O_(2) treatment in increasing CO_(2) reduction activity.The optimized Ag1.0@Ru1.0-P25 photocatalyst performed excellent CO_(2) reduction activity into CO,CH4,and C2H6 with a~95%selectivity of CH4,where the activity was~135 times higher than that of pristine TiO_(2)(P25).For the first time,this work explored the effect of H_(2)O_(2) treatment on the photocatalyst that dramatically increases CO_(2) reduction activity.

关键词： gas-phase CO_(2) reduction H_(2)O_(2) treatment plasmonic nanoparticles solar fuel photocatalyst surface modification

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Crystal structure of Arabidopsis thaliana RabA1a

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Journal of Integrative Plant Biology 2019年第2期61卷 93-109页

作者： Ji-Sook Yun Sung Chul Ha Shinae Kim Yeon-Gil Kim Hyeran Kim Jeong Ho Chang department of Biology Education Kyungpook National University beamline Science Division Pohang Accelerator Laboratory 3. Department of Biological Sciences Kangwon National University

RabGTPase is a member of the Ras superfamily of small GTPases, which share a GTP-binding pocket containing highly conserved motifs that promote GTP hydrolysis. In Arabidopsis, the RabA group, which corresponds to the Rabgroup in animals, functions in the recycling of endosomes that control docking and fusion during vesicle transport. However, their molecular mechanisms remain unknown. In this study, we determined the crystal structures of the GDP-bound inactive form and both GppNHp-and GTP-bound active forms of RabA1a, at resolutions of 2.8, 2.6, and 2.6 A?,respectively. A bound sulfate ion in the active site of the GDP-bound structure stabilized Switch Ⅱ by bridging the interaction between a magnesium ion and Arg74.Comparisons of the two states of RabA1a with Rabproteins revealed clear differences in the Switch Ⅰ and Ⅱ loops. These results suggested that conformational change of the Switch regions of RabA1a, derived by GTP or GDP binding, could maintain subcellular membrane traffic through the specific interaction of effector molecules.

关键词： GDP Crystal structure of Arabidopsis thaliana RabA Figure

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Development of a scintillating-fiber-based beam monitor for the coherent muon-to-electron transition experiment

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Nuclear Science and Techniques 2024年第4期35卷 156-164页

作者： Yu Xu Yun-Song Ning Zhi-Zhen Qin Yao Teng Chang-Qing Feng Jian Tang Yu Chen Yoshinori Fukao Satoshi Mihara Kou Oishi School of Physics Sun Yat-sen UniversityGuangzhou 510275China State Key Laboratory of Particle Detection and Electronics University of Science and Technology of ChinaHefei 230026China department of Modern Physics University of Science and Technology of ChinaHefei 230026China High Energy Accelerator Research Organization(KEK) Ibaraki 305‑0801Japan department of Physics Imperial College LondonLondon SW72AZUK

The coherent muon-to-electron transition(COMET)experiment is a leading experiment for the coherent conversion of μ^(-)N→e^(-)N using a high-intensity pulsed muon beamline,produced using innovative slow-extraction techniques.Therefore,it is critical to measure the muon beam characteristics.We set up a muon beam monitor(MBM),where scintillating fibers woven in a cross shape were coupled to silicon photomultipliers to measure the spatial profile and timing structure of the extracted muon beam for the COMET.The MBM detector was tested successfully with a proton beamline at the China Spallation Neutron Source and took data with good performance in the commissioning run.The development of the MBM,including its mechanical structure,electronic readout,and beam measurement results,are discussed.

关键词： Beam instrumentation Profile monitor Scintillating fiber Silicon photomultipliers

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Comparative evaluation for catalytic gasification of petroleum coke and asphaltene in subcritical and supercritical water

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Journal of Energy Chemistry 2019年第4期28卷 107-118页

作者： Rachita Rana Sonil Nanda Aimee Maclennan Yongfeng Hu Janusz A.Kozinski Ajay K.Dalai department of Chemical and Biological Engineering University of Saskatchewan department of Chemical and Biochemical Engineering University of Western Ontario Soft X-Ray Micro-Characterization beamline Canadian Light Source Inc. New Model in Technology & Engineering

Subcritical and supercritical water gasification of petroleum coke and asphaltene was performed at variable temperatures(350–650°C),feed concentrations(15–30 wt%)and reaction times(15–60 min).Nickel-impregnated activated carbon(Ni/AC)was synthesized as a catalyst for enhancing syngas yields at optimal gasification conditions(650°C,15 wt%and 60 min).Structural chemistry of precursors and chars developed at different gasification temperatures was studied using physicochemical and synchrotronbased approaches such as carbon–hydrogen–nitrogen–sulfur(CHNS)analysis,thermogravimetric and differential thermogravimetric analysis(TGA/DTA),scanning electron microscopy(SEM),Fourier-Transform Infrared spectroscopy(FTIR),Raman spectroscopy,X-ray diffraction(XRD)and X-ray absorption spectroscopy(XAS).Asphaltene testified to be a better precursor for catalytic hydrothermal gasification leading to 11.97 mmol/g of total gas yield compared to petroleum coke(8.04 mmol/g).In particular,supercritical water gasification using 5 wt%Ni/AC at 650°C with 15 wt%feed concentration for 60 min resulted in 4.17 and 2.98 mmol/g of H_2from asphaltene and petroleum coke,respectively.Under the same conditions,the respective CH_4yields from catalytic gasification of asphaltene and petroleum coke were 2.54and 1.07 mmol/g.Nonetheless,asphaltene also seemed to an attractive feedstock for the production of highly aromatic chars through hydrothermal gasification.

关键词： Asphaltene Petroleum coke Subcritical water Supercritical water Gasification Char

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Oxygen-deficient SnO_(2)nanoparticles with ultrathin carbon shell for efficient electrocatalytic N_(2)reduction

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Green Energy & Environment 2022年第4期7卷 672-679页

作者： Guangkai Li Haeseong Jang Zijian Li Jia Wang Xuqiang Ji Min Gyu Kim Xien Liu Jaephil Cho State Key Laboratory Base of Eco-chemical Engineering College of Chemical EngineeringCollege of Chemistry and Molecular EngineeringQingdaoUniversity of Science and TechnologyQingdao266042China department of Energy Engineering School of Energy and Chemical EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan689-798South Korea College of Materials Science and Engineering Qingdao UniversityQingdao266071China beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang790-784South Korea

For high-efficiency NH_(3)synthesis via ambient-condition electrohydrogenation of inert N_(2),it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency,good conductivity and large surface area.Here,oxygen-deficient SnO_(2)nanoparticles encapsulated by ultrathin carbon layer(d-SnO_(2)@C)are developed by hydrothermal deposition coupled with annealing process,as promising catalysts for ambient electrocatalytic N_(2)reduction.d-SnO_(2)@C exhibits high activity and excellent selectivity for electrocatalytic conversion of N_(2)to NH_(3)in acidic electrolytes,with Faradic efficiency as high as 12.7%at-0.15 V versus the reversible hydrogen electrode(RHE)and large NH_(3)yield rate of 16.68μg h^(-1)mgcat^(-1)at-0.25 V vs.RHE in 0.1 mol L^(-1)HCl.Benefiting from the structural superiority of enhanced charge transfer efficiency and optimized surface states,d-SnO_(2)@C also achieves excellent long-term stability.

关键词： N_(2)reduction reaction NH_(3)synthesis SnO_(2) Electrocatalysts Ambient conditions

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Exploring catalytic behaviors of CoS_(2)-ReS_(2) heterojunction by interfacial engineering

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Journal of Energy Chemistry 2023年第10期85卷 11-18,I0002页

作者： Jianmin Yu Yongteng Qian Sohyeon Seo Yang Liu Huong T.D.Bui Ngoc Quang Tran Jinsun Lee Ashwani Kumar Hongdan Wang Yongguang Luo Xiaodong Shao Yunhee Cho Xinghui Liu Min Gyu Kim Hyoyoung Lee department of Chemistry Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Center for Integrated Nanostructure Physics(CINAP) Institute of Basic Science(IBS)Suwon 16419Republic of Korea College of Pharmacy Jinhua PolytechnicJinhua 321007ZhejiangChina beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang University of Science and TechnologyPohang 37673Republic of Korea department of Biophysics Sungkyunkwan University2066 SeoburoJangan-guSuwon 16419Republic of Korea Creative Research Institute Sungkyunkwan University2066 SeoburoJangan-guSuwon 16419Republic of Korea

Herein, a stable and efficient CoS_(2)-ReS_(2) electrocatalyst is successfully constructed by using the different molar ratios of CoS_(2) on ReS_(2). The size and morphology of the catalysts are significantly changed after the CoS_(2) is grown on ReS_(2), providing regulation of the catalytic activity of ReS_(2). Particularly, the optimized CoS_(2)-ReS_(2) shows superior electrocatalytic properties with a low voltage of 1.48 V at 20 mA cm^(-2) for overall water splitting in 1.0 M KOH, which is smaller than the noble metal-based catalysts(1.77 V at 20 mA cm^(-2)). The XPS, XAS, and theoretical data confirm that the interfacial regulation of ReS_(2) by CoS_(2) can provide rich edge catalytic sites, which greatly optimizes the catalytic kinetics and drop the energy barrier for oxygen/hydrogen evolution reactions. Our results demonstrated that interfacial engineering is an efficient route for fabricating high-performance water splitting electrocatalysts.

关键词： CoS_(2) ReS_(2) Interfacial engineering Catalytic kinetics Water splitting

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Crystal structure of Arabidopsis thaliana RabA_(1a)

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Journal of Integrative Plant Biology 2019年第2期61卷 93-109页

作者： Ji-Sook Yun Sung Chul Ha Shinae Kim Yeon-Gil Kim Hyeran Kim Jeong Ho Chang department of Biology Education Kyungpook National University beamline Science Division Pohang Accelerator Laboratory department of Biological Sciences Kangwon National University

RabGTPase is a member of the Ras superfamily of small GTPases, which share a GTP-binding pocket containing highly conserved motifs that promote GTP hydrolysis. In Arabidopsis, the RabA group, which corresponds to the Rab_(11) group in animals, functions in the recycling of endosomes that control docking and fusion during vesicle transport. However, their molecular mechanisms remain unknown. In this study, we determined the crystal structures of the GDP-bound inactive form and both GppNHp-and GTP-bound active forms of RabA1a, at resolutions of 2.8, 2.6, and 2.6 A?,respectively. A bound sulfate ion in the active site of the GDP-bound structure stabilized Switch Ⅱ by bridging the interaction between a magnesium ion and Arg74.Comparisons of the two states of RabA1a with Rab_(11) proteins revealed clear differences in the Switch Ⅰ and Ⅱ loops. These results suggested that conformational change of the Switch regions of RabA1a, derived by GTP or GDP binding, could maintain subcellular membrane traffic through the specific interaction of effector molecules.

关键词： GDP Crystal structure of Arabidopsis thaliana RabA Figure

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