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Manipulating photogenerated electron flow in nickel single‐atom catalysts for photocatalytic CO_(2)reduction into tunable syngas

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Carbon Energy 2024年第8期6卷 205-213页

作者： Yida Zhang Qingyu Wang Lihui Wu Haibin Pan Chengyuan Liu Yue Lin Gongming Wang Xusheng Zheng national synchrotron radiation laboratory University of Science and Technology of ChinaHefeiAnhuiChina College of Chemistry and Materials science University of Science and Technology of ChinaHefeiAnhuiChina Department of Chemistry Hefei National Research Center for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefeiAnhuiChina

The key to designing photocatalysts is to orient the migration of photogenerated electrons to the target active sites rather than dissipate at inert ***,we demonstrate that the doping of phosphorus(P)significantly enriches photogenerated electrons at Ni active sites and enhances the performance for CO_(2)reduction into *** photocatalytic CO_(2)reduction,Ni single‐atom‐anchored P‐modulated carbon nitride showed an impressive syngas yield rate of 85μmol gcat^(−1)h^(−1)and continuously adjustable CO/H_(2)ratios ranging from 5:1 to 1:2,which exceeded those of most of the reported carbon nitride‐based single‐atom *** studies reveal that P doping improves the conductivity of catalysts,which promotes photogenerated electron transfer to the Ni active sites rather than dissipate randomly at low‐activity nonmetallic sites,facilitating the CO_(2)‐to‐syngas photoreduction process.

关键词： carbon nitride CO_(2)photoreduction electron flow Ni single atoms syngas

Constructing high coordination number of Ir-O-Ru bonds in IrRuO_(x)nanomeshes for highly stable acidic oxygen evolution reaction

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Nano Research 2024年第6期17卷 5073-5079页

作者： Ge Yu Ruilong Li Yida Zhang Xingen Lin Gongming Wang Xun Hong Center of Advanced Nanocatalysis(CAN) Department of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China national synchrotron radiation laboratory(NSRL) University of Science and Technology of ChinaHefei 230029China

IrRu bimetallic oxides are recognized as the promising acidic oxygen evolution reaction(OER)catalysts,but breaking the trade-off between their activity and stability is an unresolved ***,addressing the issues of mass transport obstruction of IrRu bimetallic oxides under high current remains a challenge for the development of proton exchange membrane water electrolysis(PEM-WE).Herein,we prepared an IrRuO_(x)nanomeshes(IrRuO_(x)NMs)with high coordination number(CN)of Ir-O-Ru bonds in a mixed molten salt with high solubility of the Ir/Ru precursor.X-ray absorption spectroscopy analysis revealed that the IrRuO_(x)NMs possess high coordination number of Ir-O-Ru bonds(CNIr-O-Ru=5.6)with a distance of 3.18Å.Moreover,the nanomesh structures of IrRuO_(x)NMs provided hierarchical channels to accelerate the transport of oxygen and water,thus further improving the electrochemical ***,the IrRuO_(x)NMs as OER catalysts can simultaneously achieve high activity and stability with low overpotential of 196 mV to reach 10 mA·cm^(−2)and slightly increase by 70 mV over 650 h *** electrochemical mass spectrometry tests suggest that the preferred OER mechanism for IrRuO_(x)NMs is the adsorbent evolution mechanism,which is beneficial for the robust structural stability.

关键词： oxygen evolution reaction IrRuO_(x) Ir-O-Ru bonds two-dimensional(2D)nanomesh proton exchange membrane device mass transport

Classical spin liquid state in a rhombic lattice metal-organic framework

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Nano Research 2024年第4期17卷 3407-3412页

作者： Sihua Feng Chao Wang Jiyin Zhao Xuguang Liu Chaocheng Liu Zeming Qi Lei Chen Huijuan Wang Minghui Fan Hengli Duan Wensheng Yan national synchrotron radiation laboratory University of Science and Technology of ChinaHefei 230026China hefei national Research Center for Physical sciences at the Microscale University of Science and Technology of ChinaHefei 230026China School of Materials science and Engineering Hefei University of TechnologyHefei 230009China Experimental Center of Engineering and Material science University of Science and Technology of ChinaHefei 230026China

Discovering more and new geometrically frustrated systems remains an active point of inquiry in fundamental physics for the existence of unusual states of ***,we report spin-liquid-like behavior in a two-dimensional(2D)rhombic lattice Fe-metal-organic framework(Fe-MOF)with frustrated *** Fe-MOF exhibits a high frustration factor f=|θCW|/TN≥315,and its long-range magnetic order is suppressed down to 180 *** theoretical calculations demonstrate strong antiferromagnetic coupling between adjacent Fe3+ions,indicating the potential of a classical spin-liquid-like ***,a T-linear heat capacity parameter,γ,originating from electronic contributions and with magnetic field independence up to 8 T,can be observed in the specific heat capacity measurements at low-temperature,providing further proof for the spin-liquid-like *** work highlights the potential of MOF materials in geometrically frustrated systems,and will promote the research of exotic quantum physics phenomena.

关键词： spin-liquid-like state two-dimensional metal-organic framework(2D MOF) rhombic lattice ultralow temperature(ULT)measurements spin-frustrated

Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction

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science china Chemistry 2024年第4期67卷 1352-1359页

作者： Tong Liu Yudan Chen Airong Xu Xiaokang Liu Dong Liu Sicheng Li Hui Huang Li Xu Shuaiwei Jiang Qiquan Luo Tao Ding Tao Yao national synchrotron radiation laboratory University of Science and Technology of ChinaHefei 230029China Key laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei 230026China Institutes of Physical science and Information technology Anhui UniversityHefei 230601China

Exploring the atomic interaction mechanisms of dense single-atom catalysts(SACs)is of great significance for their application in oxygen reduction reaction(ORR).However,the intrinsic mechanism of the site-distance effect on the catalytic performance has been largely ***,we demonstrate the site-distance effect of Fe-Rh_(x)@NC catalysts in ORR theoretically and *** charge analysis reveals that the strong interaction between Fe and Rh atoms at a certain atomic distance(dFe-Rh)alters the catalytic electronic structure,facilitating the optimization of catalyst adsorption *** by the theoretical calculations,we designed and synthesized the Fe-Rhx@NC catalysts through a spatial confinement *** characterization results prove that the Fe-Rh_(2)@NC has the optimal d_(Fe-Rh),which improves its intrinsic ORR activity,providing a half wave potential of 0.91 V,higher than that of the commercial Pt/C(0.86 V).This study emphasizes the importance of determining the basic mechanism of the site-distance effect in dissimilar metal atoms catalysts,which is conducive to the design of efficient catalyst systems for practical applications.

关键词： Density functional theory single-atom catalyst in-situ encapsulating site-distance effect oxygen reduction reaction

Quick-scanning X-ray absorption fine structure beamline at SSRF

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Nuclear science and Techniques 2024年第6期35卷 1-13页

作者： Yu Chen Qian Gao Zheng Jiang Jiong Li Shuo Zhang Shanghai synchrotron radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China national synchrotron radiation laboratory University of Science and Technology of ChinaHefei 230029China

The layout and characteristics of the hard X-ray spectroscopy beamline(BL11B)at the Shanghai synchrotron radiation facility are described ***11B is a bending-magnet beamline dedicated to conventional and millisecond-scale quick-scanning X-ray absorption fine *** is equipped with a cylindrical collimating mirror,a double-crystal monochromator comprising Si(111)and Si(311),a channel-cut quick-scanning Si(111)monochromator,a toroidal focusing mirror,and a high harmonics rejection *** can provide 5-30 keV of X-rays with a photon flux of~5×10^(11)photons/s and an energy resolution of~1.31×10^(-4)at 10 *** performance of the beamline can satisfy the demands of users in the fields of catalysis,materials,and environmental *** paper presents an overview of the beamline design and a detailed description of its performance and capabilities.

关键词： Bending magnet beamline X-ray absorption fine structure Quick-scanning XAFS In situ synchrotron radiation

Surface-sensitive electronic structure of kagome superconductor CsV_(3)Sb_(5)

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Chinese Physics B 2024年第10期33卷 35-40页

作者： Zhisheng Zhao Jianghao Yao Rui Xu Yuzhe Wang Sen Liao Zhengtai Liu Dawei Shen Shengtao Cui Zhe Sun Yilin Wang Donglai Feng Juan Jiang School of Emerging technology and Department of Physics University of Science and Technology of ChinaHefei 230026China Shanghai synchrotron radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China national synchrotron radiation laboratory School of Nuclear science and technology and New Cornerstone Science LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

We systematically study the electronic structure of a kagome superconductor CsV_(3)Sb_(5)at different temperatures coveringboth its charge density wave state and normal state with angle-resolved photoemission *** observe thatthe V-shaped band aroundГshows three different behaviors,referred to as a/a',βandγ,mainly at different *** investigations confirm that these bands are all from the same bulk Sb-p_(z)origin,but they are quite sensitiveto the sample surface conditions mainly modulated by ***,the intriguing temperature dependent electronicbehavior of the band nearГis affected by the sample surface condition,rather than intrinsic electronic behavior originatingfrom the phase *** result systematically reveals the confusing electronic structure behavior of the energy bandsaroundГ,facilitating further exploration of the novel properties in this material.

关键词： kagome ARPES charge density wave surface sensitive

Atomically precise Ru-O-Ru clusters for enhanced water dissociation in alkaline hydrogen evolution

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Nano Research 2024年第8期17卷 6993-7000页

作者： Dong Liu Li Xu Sicheng Li Airong Xu Yuanhua Sun Tong Liu Mengyuan Liu Huijuan Wang Xiaokang Liu Tao Yao Tao Ding hefei national Research Center for Physical sciences at the Microscale School of Nuclear Science and TechnologyKey Laboratory of Precision and Intelligent ChemistryNational Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230029China Experimental Center of Engineering and Materials science University of Science and Technology of ChinaHefei 230026China

Atomic clusters typically exhibit distinctive electronic structures and physicochemical ***,as the size decreases,their ability to adsorb and dissociate water also diminishes,thereby affecting chemical reactions involving water *** the adsorption and dissociation capabilities of atomic clusters towards water molecules and elucidating the mechanisms underlying their performance enhancement have become important research ***,employing the carrier-anchored strategy,Ru-O-Ru atomic clusters were prepared and displayed excellent activity and durability in the hydrogen evolution ***,the Ru-O-Ru atomic clusters exhibited only 86 mV overpotential at 100 mA·cm−^(2) and superior membrane-electrode-assembly activity than commercial Ru/C *** radiation-based Fourier transform infrared spectroscopic measurements revealed that the modification of oxygen in Ru-O-Ru units promoted the reorientation of water molecules from a H-up orientation to H-down,therefore,enhanced the formation of strong hydrogen-bond network of interfacial water on the surface of Ru-O-Ru clusters,leading to enhanced adsorption and dissociation of water and accelerated Volmer *** findings provide a potential strategy and deep insights for the development of atomic clusters in electrocatalysts.

关键词： hydrogen evolution in-situ Fourier transform infrared(FTIR) Ru catalysts electrocatalysis atomic clusters

Low-coordination environment design of single Co atoms for efficient CO_(2) photoreduction

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Nano Research 2024年第5期17卷 3745-3751页

作者： Zhentao Ma Qingyu Wang Limin Liu Rong-Ao Zhang Qichen Liu Peigen Liu Lihui Wu Chengyuan Liu Yu Bai Yida Zhang Haibin Pan Xusheng Zheng national synchrotron radiation laboratory University of Science and Technology of ChinaHefei 230029China College of Chemistry and Materials science University of Science and Technology of ChinaHefei 230026China Experimental Center of Engineering and Material science University of Science and Technology of ChinaHefei 230026China

Photocatalytic carbon dioxide(CO_(2))to carbon monoxide(CO)offers a promising way for both alleviating the greenhouse effect and meeting the industrial ***,we constructed a Co single-atom catalyst with intentional low-coordination environment design on porous ZnO(denoted as Co1/ZnO).Impressively,Co1/ZnO exhibited a remarkable activity with a CO yield rate of 22.25 mmol·g^(-1)·h^(-1) and a selectivity of 80.2%for CO_(2) photoreduction reactions under visible *** incorporation of single Co atoms provided an additional photo-generated electron transfer channel,which suppressed the carrier recombination of ***,the unsaturated Co active sites were capable to adsorb CO_(2) molecule spontaneously,thus facilitating the activation of CO_(2) molecule during CO_(2) reduction course.

关键词： photocatalytic CO_(2)reduction single atoms low-coordination CO_(2)adsorption electron transfer

Beam based alignment using a neural network

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Nuclear science and Techniques 2024年第4期35卷 108-118页

作者： Guan-Liang Wang Ke-Min Chen Si-Wei Wang Zhe Wang Tao He Masahito Hosaka Guang-Yao Feng Wei Xu national synchrotron radiation laboratory University of Science and Technology of ChinaHefei 230029China Diamond Light Source Oxfordshire OX110DEUK

Beams typically do not travel through the magnet centers because of errors in storage *** beam deviating from the quadrupole centers is affected by additional dipole fields due to magnetic field ***-based alignment(BBA)is often performed to determine a golden orbit where the beam circulates around the quadrupole center *** storage rings with many quadrupoles,the conventional BBA procedure is time-consuming,particularly in the commissioning phase,because of the necessary iterative *** addition,the conventional BBA method can be affected by strong coupling and the nonlinearity of the storage ring *** this study,a novel method based on a neural network was proposed to determine the golden orbit in a much shorter time with reasonable *** golden orbit can be used directly for operation or adopted as a starting point for conventional *** method was demonstrated in the HLS-II storage ring for the first time through simulations and online *** results of the experiments showed that the golden orbit obtained using this new method was consistent with that obtained using the conventional *** development of this new method and the corresponding experiments are reported in this paper.

关键词： Golden orbit Beam-based alignment Neural network Storage ring