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Highly efficient photocatalytic conversion of CO_(2) into CH_(4) over Cu single atom promoted heterojunction:The effect of uplifted d-band center

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Chinese Chemical Letters 2024年第2期35卷 484-488页

作者： Hao Zhang Qian Liu Zhurui Shen School of Materials Science and Engineering Nankai UniversityTianjin 300350China

Photoreduction of CO_(2) to solar fuels has caused great interest,but suffers from low catalytic efficiency and poor ***,we designed a S-scheme heterojunction(Cu-TiO_(2)/WO_(3))with Cu single atom to significantly boost the photoreduction of CO_(2).Notably,the developed Cu-TiO_(2)/WO_(3) achieved the solardriven conversion of CO_(2) to CH_(4) with an evolution rate of 98.69μmol g^(−1) h^(−1),and the electron selectivity of CH_(4) reached 88.5%.The yield was much higher than those of pristine WO_(3),TiO_(2)/WO_(3) and Cu-TiO_(2) *** and theoretical analysis suggested that the S-scheme heterojunction accelerated charge migration and inhibited the recombination of electron-hole ***,the charge separation effect of the heterojunction meliorated the position of the *** uplifted d-band centers of Cu and Ti on Cu-TiO_(2)/WO_(3) not only improved the electron interaction between Cu single atoms and substrate-TiO_(2),accelerated the adsorption and activation of CO_(2) on the active sites of Cu single atom,but also optimized the Gibbs free energies of CH 4 formation pathway,leading to excellent selectivity toward CH_(4).This work provides new insights into the design of photocatalyst systems with high photocatalytic performance.

关键词： Cu single atom Heterojunction CO_(2)photoreduction d-band center dFT

Tailoring d-band center over electron traversing effect of Ni M@C-CoP(M=Zn,Mo,Ni,Co)for high-performance electrocatalysis hydrogen evolution

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Journal of Materials Science & Technology 2023年第35期166卷 164-172页

作者： Hao Luo Xudong Zhang Hui Zhu Kexin Zhang Fan Yang Kewei Xu Sen Yu dagang Guo State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and EngineeringXi’an Jiaotong UniversityXi’an710049China center for High Performance Computing Network Information CenterXi’an Jiaotong UniversityXi’an710049China State Key Laboratory for Manufacturing Systems Engineering Xi’an Jiaotong UniversityXi’an710049China Shaanxi Key Laboratory of Biomedical Metal Materials Northwest Institute for Non-ferrous Metal ResearchXi’an710016China

Attaining a highly efficient and inexpensive electrocatalyst is significant for the hydrogen evolution reaction(HER)but still challenging *** transition-metal phosphides(TMPs)catalysts with platinum-like electronic structures are a potential candidate for the HER,but those are prone to be strongly bound with hydrogen intermediates(H∗),resulting in sluggish HER *** we report a unique hybrid structure of CoP anchored on graphene nanoscrolls@carbon nano tubes(CNTs)scaffold(Ni M@C-CoP)encapsulating various Ni M(M=Zn,Mo,Ni,Co)bimetal nanoalloy via chemical vapor deposi-tion(CVd)growth of CNT on graphene nanoscrolls followed by the impregnation of cobalt precursors and phosphorization for efficiently electrocatalytic hydrogen *** nanoparticles mainly scattered at the tip of CNT branches which exhibited the analogical“Three-layer core-shell”*** and density functional theory(dFT)calculations consistently disclose that the encapsulated various NiMs can offer different numbers of electrons to weaken the interactions of outmost CoP with H∗and push the downshift of the d-band center to different degrees as well as stabilize the outmost CoP nanopar-ticles to gain catalytic stability via the electron traversing *** electrocatalytic HER activity can be maximumly enhanced with low overpotentials of 78 mV(alkaline)and 89 mV(acidic)at a current density of 10 mA/cm^(2) and sustained at least 24 h especially for NiZn@C-CoP *** novel system is distinct from conventional three-layer heterostructure,providing a specially thought of d-band center control engineering strategy for the design of heterogeneous catalysts and expanding to other electrocat-alysts,energy storage,sensing,and other applications.

关键词： Electron traversing effect 3d graphene/CNT CoP nanoparticle d-band center Hydrogen evolution

General strategy for evaluating the d-band center shift and ethanol oxidation reaction pathway towards Pt-based electrocatalysts

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Science China Chemistry 2023年第1期66卷 279-288页

作者： Jin-Hong Zheng Guang Li Jun-Ming Zhang Ningyan Cheng Li-Fei Ji Jian Yang Jialin Zhang Bin-Wei Zhang Yan-Xia Jiang Shi-Gang Sun State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing 400044China Key Laboratory of Magnetic Molecules&Magnetic Information Materials Ministry of Education School of Chemical and Material ScienceShanxi Normal UniversityTaiyuan 030031China Information Materials and Intelligent Sensing Laboratory of Anhui Province Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationInstitutes of Physical Science and Information TechnologyAnhui UniversityHefei 230039China

The catalytic performance of Pt-based catalysts depends sensitively on their d-band ***,there are still huge challenges to evaluate their d-band centers from experimental technologies,and modulate them to analyze their selectivity in ethanol oxidation reaction(EOR).Here,Pt1Au1alloy supported on the commercial carbon material(Pt_(1)Au_(1)/C)is employed as a typical example to investigate its d-band center shift of surface Pt,and as electrocatalysts to study its selectivity towards ***,a highly reliable in situ Fourier-transform infrared spectroscopy CO-probe strategy is developed to characterize the d-band center shift of surface *** modified electronic effect and site effect of Pt_(1)Au_(1)/C dictated the adsorption configuration of intermediate species and the OH species coverage,thereby influencing its *** importantly,we developed a universal cyclic voltammetry peak differentiation fitting method as an electrochemical analysis technique to investigate CO_(2)selectivity,which is potentially extendable to other Pt-based electrocatalysts.

关键词： PtAu in situ FTIRS d-band center ethanol oxidation reaction CV peak differentiation fitting method

基于配体效应协同调控异质结氧化还原位点的d带中心用于光解水制氢

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Science China Materials 2024年第2期67卷 524-531页

作者：吴园霄曲梦茹姜淑娟张建军宋少青 School of Materials Science&Chemical Engineering Ningbo UniversityNingbo 330013China School of New Energy Ningbo University of TechnologyNingbo 315336China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China

光催化水解离制氢过程中,光生载流子由生成位点向氧化还原位点艰难的动力学迁移及随后与中间产物反应大的过电位问题还没有被解决,严重阻碍了太阳光子转化为氢能的效率(STH).本文基于配体效应协同调控材料d带中心构建了CeO_(2)纳米线负... 详细信息

光催化水解离制氢过程中,光生载流子由生成位点向氧化还原位点艰难的动力学迁移及随后与中间产物反应大的过电位问题还没有被解决,严重阻碍了太阳光子转化为氢能的效率(STH).本文基于配体效应协同调控材料d带中心构建了CeO_(2)纳米线负载Ni_(2)P异质结光催化剂,继而解决上述动力学瓶颈.原位漫反射傅里叶变换红外光谱、霍尔效应等表征揭示光生电子和空穴在自发局域电场推动下,分别迁移至Ni_(2)P还原位点和CeO_(2)氧化位点,接着促使吸附在此的活性中间产物发生脱氢和氧耦合反应.性能测试显示,在AM 1.5G模拟太阳光辐照下,室温下的STH值达到了1.13%.本研究为通过协同调节d带中心提高异质结光催化剂的STH提供了独特的策略.

关键词： heterojunction d-band center H_(2)O splitting H_(2)energy photocatalysis

Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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Carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State Key Laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

Modulation of d-orbital to realize enriched electronic cobalt sites in cobalt sulfide for enhanced hydrogen evolution in electrocatalytic water/seawater splitting

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Rare Metals 2024年第2期43卷 511-521页

作者： Jian-Peng Sun Yu Zheng Zi-Sheng Zhang Xiang-Chao Meng Zi-Zhen Li Key Laboratory of Marine Chemistry Theory and Technology(Ministry of Education) College of Chemistry and Chemical EngineeringOcean University of ChinaQingdao266100China Shanxi Institute of Energy Taiyuan030600China department of Chemical and Biological Engineering Faculty of EngineeringUniversity of OttawaOttawaONK1N6 N5Canada

Herein,a novel single-atomic Pt doping and interface-rich CoS/Co(OH)_(2)(Pt-CoS/Co(OH)_(2)/C)electrocatalyst has been successfully *** from precise regulation of d-orbital electronic structure modulation on Co site,Pt-CoS/Co(OH)_(2)/C exhibited remarkable HER activity and high stability for hydrogen evolution in splitting both water(73 mV@10 mA·cm^(−2)) and seawater(87 mV@10 mA·cm^(−2)).Notably,atomic Pt doping was introduced into CoS/Co(OH)_(2),which could produce local unbalanced Coulombic force and significantly increased the number of S vacancies,and then expose abundant Co ***,Co(OH)_(2) in Pt-CoS/Co(OH)_(2)/C could act as the adsorption sites for H_(2)O in hydrogen evolution reaction *** functional theory results also proved that atomic Pt doping,S vacancies and Co(OH)_(2) coupling could result in the formation of enriched electronic Co sites and optimize d_(z2) orbital electronic structure,and then realize the depth upward shift of d-band center and enhance the adsorption of H*on Co sites.

关键词： Electrocatalysts Hydrogen evolution reaction Pt-CoS/Co(OH)_(2) d-band center Electronic structure Water/seawater electrolysis

Boosting overall saline water splitting by constructing a strain-engineered high-entropy electrocatalyst

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Carbon Energy 2024年第2期6卷 154-166页

作者： Ateer Bao Yaohang Gu Yuxuan Zhang Bowen Zhang Juncheng Wu Bo Ni Xiaoyan Zhang Haijun Pan Xiwei Qi School of Materials Science and Engineering Northeastern UniversityShenyangChina School of Resources and Materials Northeastern University at QinhuangdaoQinhuangdaoChina Key Laboratory of dielectric and Electrolyte Functional Material Hebei Province Northeastern University at QinhuangdaoQinhuangdaoChina College of Metallurgy and Energy North China University of Science and TechnologyTangshanChina

High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent ***,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic *** confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical ***,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,*** strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water ***,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.

关键词： d-band center electrical conductivity high-entropy electrocatalyst lattice-strain engineering saline/alkaline water splitting

Understanding the Pt-like Catalytic Activity of Transition Metal Carbide Ta4C_(3) for I_(3)^(-) Reduction

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材料科学与工程（中英文A版） 2024年第1期14卷 18-25页

作者： Jing Li Rui Yu Yingchun Li School of Materials Science&Engineering North University of ChinaTaiyuan 030051Shanxi ProvincePR China School of Materials Science and Engineering Beihang UniversityBeijing 100191PR China

This paper attempts to understand the Pt-like catalytic activity of transition metal carbide Ta4C_(3) for IRR(I_(3)^(-)reduction reaction)based on the correlation of adsorption energy to d-band center(εd).Ta4C_(3) was prepared by carbothermal reduction method with a *** photoelectrochemical properties were investigated as a CE(counter electrode)in dSSC(dye-sensitized solar cell).Its surface electronic structures,including dOS(density of state)andεd,and adsorption energy were computed by first-principle dFT(density functional theory).In TMC(transition metal carbide)Ta4C_(3),the interaction between Ta and C atoms makes the d-band of Ta broaden and results in the downward shift of itsεd.A moderate absorption energy corresponding to theεd is achieved,which is the nature of the Pt-like catalytic activity of Ta4C_(3).Appropriate change of adsorption energy by adjustingεd is a promising strategy to improve catalytic *** work is of great significance to the fundamental and application researches.

关键词： Pt-like catalytic activity Ta4C_(3) dOS d-band center absorption energy.

Selective and effective oxidation of 5-hydroxymethylfurfural by tuning the intermediates adsorption on Co-Cu-CN_(x)

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Nano Research 2023年第5期16卷 6670-6678页

作者： Tianyun Jing Shaokang Yang Yonghai Feng Tingting Li Yunpeng Zuo dewei Rao School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China Institute of Surface Micro and Nano Materials Xuchang UniversityXuchang 461002China Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research InstitutePalackýUniversity77900 OlomoucCzech Republic Pharmaceutical Sciences Laboratory and Turku Bioscience center Åbo Akademi UniversityTurku 20520Finland

Co-based catalysts are promising alternatives to precious metals for the selective and effective oxidation of 5-hydroxymethylfurfural(HMF)to the higher value-added 2,5-furandicarboxylic acid(FdCA).However,these catalysts still suffer from unsatisfactory activity and poor selectivity.A series of N-doped carbon-supported Co-based dual-metal nanoparticles(NPs)have been designed,among which the Co-Cu_(1.4)-CN_(x) exhibits enhanced HMF oxidative activity,achieving FdCA formation rates 4 times higher than that of pristine Co-CN_(x),with 100%FdCA *** functional theory(dFT)calculations evidenced that the increased electron density on Co sites induced by Cu can mediate the positive electronegativity offset to downshift the dband center of Co-Cu_(1.4)-CN_(x),thus reducing the energy barriers for the conversion of HMF to *** findings will support the development of superior non-precious metal catalysts for HMF oxidation.

关键词： Co-based materials 5-hydroxymethylfurfural(HMF)oxidative activity 2,5-furandicarboxylic acid(FdCA)selectivity electronegativity offset d-band center