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Operando HERFD-XANES and surface sensitive Δμ analyses identify the structural evolution of copper(Ⅱ) phthalocyanine for electroreduction of CO_(2)

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Journal of Energy Chemistry 2022年第1期31卷 1-7,I0001页

作者： Bingbao Mei Cong Liu Ji Li songqi gu Xianlong Du Siyu Lu Fei Song Weilin Xu Zheng Jiang Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Electroanalytical Chemistry &Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China College of Chemistry College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450000HenanChina Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China

The quantitative understanding of how atomic-level catalyst structural changes affect the reactivity of the electrochemical CO_(2)reduction reaction is *** to the complexity of catalytic systems,conventional in situ X-ray spectroscopy plays a limited role in tracing the underlying dynamic structural changes in catalysts active ***,operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy was used to precisely identify the dynamic structural transformation of well-defined active sites of a representative model copper(Ⅱ)phthalocyanine catalyst which is of guiding significance in studying single-atom catalysis *** X-ray spectroscopy analyses,including surface sensitive△μspectra which isolates the surface changes by subtracting the disturb of bulk base and X-ray absorption near-edge structure spectroscopy simulation,were used to discover that Cu species aggregated with increasing applied potential,which is responsible for the observed evolution of C_(2)H_(4).The approach developed in this work,characterizing the active-site geometry and dynamic structural change,is a novel and powerful technique to elucidate complex catalytic mechanisms and is expected to con tribute to the rational design of highly effective catalysts.

关键词： Operando HERFD-XANES △μanalysis Structural evolution Copper(Ⅱ)phthalocyanine Electrochemical CO_(2)reduction reaction

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Effects of cobalt carbide on Fischer–Tropsch synthesis with MnO supported Co-based catalysts

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Journal of Energy Chemistry 2020年第3期29卷 227-232页

作者： Fanfei Sun Ruoou Yang Zhaoming Xia Yuqi Yang Ziang Zhao songqi gu Dongshuang Wu Yunjie Ding Zheng Jiang Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China Shanghai Synchrotron Radiation Facility Zhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100100China Center for Applied Chemical Research Frontier Institute of Science and TechnologyXi’an Jiaotong UniversityXi’an 710049ShaanxiChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Graduate school of science Kyoto UniversityKitashirakawaOiwake-choSakyo-kuKyoto-shiKyoto-fu606-8502Japan

Cobalt carbide(Co2C)was considered as potential catalysts available for large-scale industrialization of transforming syngas(H2 and CO)to clean ***,we successfully synthesized Co-based catalysts with MnO supported,to comprehend the effects of Co2C for Fischer–Tropsch synthesis(FTS)under ambient *** huge variety of product selectivity which was contained by different active sites(Co and Co2C)has been ***,density functional theory(DFT)shows that Co2C is efficacious of CO adsorption,whereas is weaker for H adsorption than *** the advantages of Co and Co2C,the catalyst herein can not only obtain more C5+products but also suppress methane *** can be a commendable guide for the design of industrial application products in FTS.

关键词： Cobalt carbide Fischer–Tropsch synthesis X-ray absorption fine spectroscopy nanomaterials Density functional theory

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Characterization of CoMn catalyst by in situ X-ray absorption spectroscopy and wavelet analysis for Fischer–Tropsch to olefins reaction

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Journal of Energy Chemistry 2019年第5期28卷 118-123页

作者： Ruoou Yang Zhaoming Xia Ziang Zhao Fanfei Sun Xianlong Du Haisheng Yu songqi gu Liangshu Zhong Jingtai Zhao Yunjie Ding Zheng Jiang Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China School of Materials Science and Engineering Shanghai UniversityShanghai 200444China Center for Applied Chemical Research Frontier Institute of Science and TechnologyXi'an Jiaotong UniversityXi'an 710049ShaanxiChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201203China

Cobalt carbide has recently been reported to catalyse the FTO con version of syngas with high selectivity for the production of lower olefins (C2-C4). Clarifying the formation process and atomic structure of cobalt carbide will help understand the catalytic mechanism of FTO. Herein, hydrogenati on of carb on monoxide was investigated for cobalt carbide synthesized from CoMn catalyst, followed by X-ray diffraction, transmission electron microscopy, temperature programmed reaction and in situ X-ray absorption spectroscopy. By monitoring the evolution of cobalt carbide during syngas conversion, the wavelet transform results give evidenee for the formation of the cobalt carbide and clearly demonstrate that the active site of catalysis was cobalt carbide.

关键词： In situ XAFS Wavelet transform Cobalt carbide FTO

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Role of local coordination in bimetallic sites for oxygen reduction: A theoretical analysis

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Journal of Energy Chemistry 2020年第5期29卷 131-137页

作者： Yuqi Yang Hao Zhang Zhaofeng Liang Yaru Yin Bingbao Mei Fei Song Fanfei Sun songqi gu Zheng Jiang Yuen Wu Zhiyuan Zhu Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China Shanghai Synchrotron Radiation Facility Zhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China Department of Chemistry Hefei National Laboratory for Physical Sciences at the MicroscaleiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)University of Science and Technology of ChinaHefei 230026AnhuiChina ShanghaiTech University Shanghai 201210China

Understanding of the oxygen reduction reaction(ORR)mechanism for single atom catalysts is pivotal for the rational design of non-precious metal cathode materials and the commercialization of fuel ***,a series of non-precious metal electrocatalysts based on nitrogen-doped bimetallic(Fe and Co)carbide were modeled by density functional theory calculations to predict the corresponding reaction *** study elucidated prior oxygen adsorption on the Fe atom in the dual site and the modifier role of Co atoms to tune the electronic structures of *** reaction activity was highly correlated with the bimetallic center and the coordination environment of the adjacent ***,the preadsorption of*OH resulted in the apparent change of metal atoms'electronic states with the d-band center shifting toward the Fermi level,thereby boosting reaction *** result should help promote the fundamental understanding of active sites in ORR catalysts and provide an effective approach to the design of highly efficient ORR catalysts on an atomic scale.

关键词： Non-precious metal catalysts Bimetallic-sites Oxygen reduction reaction Density functional theory

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Unveiling the mechanism of charge compensation in Li_(2)Ru_(x)Mn_(1-x)O_(3)by tracking atomic structural evolution

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Journal of Energy Chemistry 2022年第12期75卷 267-275,I0007页

作者： Ji Li Hongzhou Liu Shun Zheng Yande Li Daming Zhu Fanfei Sun Jingyuan Ma songqi gu Panzhe Qiao Shuai Yang Xianlong Du Xiaosong Liu Zhi Liu Bingbao Mei Zheng Jiang Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China University of Chinese Academy of Sciences Beijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Shanghai Institute of Microsystem and Information Technology Chinese Academy of SciencesShanghai 200050China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina

The relationship between the structural evolution and redox of Li-rich transition-metal layered oxides(LLOs)cathodes remains ambiguous,obstructing the development of high-performance lithium-ion(Li^(+))***,the coherent effects of local atomic and electronic structure in Li_(2)Ru_(x)Mn_(1-x)O_(3)(LRMO)with a wide voltage window(1.3–4.8 V)is identified by in situ X-ray absorption fine spectroscopy(XAFS)and *** not only skillfully separated the redox active structures to track the electrochemical path,but also visualized the coupling mechanism between the evolution of Ru-Ru dimer and the(de)excitation of cations and ***,introducing manganese triggers the“heterogeneity”of coordination environment and electronic structure between Ru and Mn after discharge to 3 *** change of thermodynamic and kinetic paths affects the relithiation,and further leads to the hysteresis of the anion activation structure relaxation of Li_(2)Ru_(0.4)Mn_(0.6)O_(3)relative to Li_(2)RuO_(3)(LRO).Additionally,it is demonstrated that the high charge cut-off voltage restrains the relaxation of anionic active structure in LRO from a new perspective through comparative *** work associates the evolution of atomic structure with charge compensation and negative electrochemical reactions such as voltage hysteresis(VH)and capacity attenuation,deepening the understanding electrochemical reaction mechanism of LLOs during the first cycle and providing a theoretical support for the further design and synthesis of high-efficiency cathodes.

关键词： Li-rich transition-metal layered oxides In situ XAFS Ru-Ru dimer Atomic structure Charge compensation

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基于PILATUS探测器的von Hamos构型X射线发射谱谱仪及数据获取

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核技术 2022年第9期45卷 1-7页

作者：顾颂琦梅丙宝姜政黄宇营中国科学院上海应用物理研究所上海201800 中国科学院上海高等研究院上海201204 中国科学院大学北京100049

高能量分辨X射线发射谱(X-ray Emission Spectroscopy,XES)比常规X射线吸收精细结构谱(X-ray Absorption Fine Structure,XAFS)具有更高的能量分辨率,是探究物质精细电子结构的有力工具。PILATUS探测器是一种没有暗电流和读出噪声的单... 详细信息

高能量分辨X射线发射谱(X-ray Emission Spectroscopy,XES)比常规X射线吸收精细结构谱(X-ray Absorption Fine Structure,XAFS)具有更高的能量分辨率,是探究物质精细电子结构的有力工具。PILATUS探测器是一种没有暗电流和读出噪声的单光子计数探测器,基于该探测器,在上海光源BL14W1线站搭建了一套von Hamos构型XES谱仪及数据获取系统,能量分辨率达到eV量级,接近此类构型光谱仪的世界先进水平。该光谱仪采用PILATUS探测器作为位置灵敏探测器使用,并结合线站单色器和KOHZU平台系统开发了一套基于LabVIEW软件的XES数据获取系统。对光谱仪系统进行了能量分辨率测试和CuO发射谱测量实验,获得样品发射的能量为8046 eV弹性散射峰的半高宽(Full-Widthat Half Maximum,FWHM)为1.67 eV,表明基于PILATUS探测器的von Hamos构型XES谱仪系统可以满足高能量分辨实验的需求。

关键词： PILATUS 高能量分辨X射线发射谱 von Hamos 数据获取

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试论中学教师继续教育课程设置

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当代教育论坛 2006年第2期 106-107页

作者：顾松麒湖南省中小学教师继续教育指导中心主任、特级教师、副教授

课程设置是教师继续教育工作的关键一环,也是培训工作的核心内容.在设置中学教师继续教育课程时,必需适应基础教育改革和发展的要求,结合在职教师的实际情况,以促进教师自身专业发展为目的,全面构建继续教育的课程体系.

关键词：教师继续教育课程设置课程目标在职培训就业后培训教师职业道德教师队伍师资队伍中学中等学校

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上海光源BL14W1线站透射XAFS数据采集系统升级

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核技术 2022年第7期45卷 27-35页

作者：刘泓舟李季顾颂琦苏晓智梅丙宝姜政刘志上海科技大学上海201210 中国科学院上海应用物理研究所上海201800 中国科学院大学北京100049 中国科学院上海高等研究院上海光源科学中心上海201204

X射线吸收光谱(X-ray Absorption Spectroscopy,XAS)在材料科学、生物学、化学等领域有着广泛的应用。为了提高上海光源BL14W1光束线站同步辐射X射线吸收精细结构谱(X-ray Absorption Fine Structure spectroscopy,XAFS)的透射数据采集... 详细信息

X射线吸收光谱(X-ray Absorption Spectroscopy,XAS)在材料科学、生物学、化学等领域有着广泛的应用。为了提高上海光源BL14W1光束线站同步辐射X射线吸收精细结构谱(X-ray Absorption Fine Structure spectroscopy,XAFS)的透射数据采集的效率,搭建了基于分布式数据采集节点和XAFS测试多样品架的数据采集系统。分布式数据采集节点采用了集成式设计,开放了底层系统,能够直接获取电压信号和编码器信号,并具有体积小、噪音小、成本低、易于维护等优点;XAFS测试多样品架提供了12个样品孔位,并可以远程控制其孔位切换。将两个硬件设备相结合搭建出新型数据采集系统,并提供了多样品自动筛选采谱的功能。采用LabVIEW编写的新数据采集系统与自动筛选采谱程序实现了多样品XAFS的自动筛选及高信噪比自动采集,大大提高了数据采集的效率,为整个线站的运行带来采谱效率大幅提高、成本降低、维护难度降低、占用空间减小等多方面的提升。

关键词：同步辐射数据采集 X射线吸收精细结构谱 LabVIEW

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基于LabVIEW的高能量分辨谱仪数据采集系统

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核技术 2017年第10期40卷 7-12页

作者：顾颂琦段佩权张硕姜政黄宇营李炯中国科学院上海应用物理研究所嘉定园区上海201800

在上海光源BL14W1线站,成功搭建一套基于Lab VIEW的高能量分辨谱仪运动控制和数据采集系统,该光谱仪系统可以实现高能量分辨荧光探测X射线吸收谱(High Energy Resolution Fluorescence Detected X-ray Absorption Spectroscopy,HERFD-XAS)、X射线发射谱(X-ray Emission Spectroscopy,XES)和共振X射线发射谱(Resonant X-ray Emission Spectroscopy,RXES)等主要实验功能,分辨率达到亚电子伏。硬件系统采用上海光源统一的VME运动控制硬件系统和硅漂移固体探测器;软件系统采用Lab VIEW编写用户操作界面,利用DSC(Data logging and Supervisory Control Module)模块实现与运动控制使用的实验与物理工业控制系统(Experimental and Physics Industrial Control System,EPICS)系统的数据交换。利用基于该运动控制和数据采集系统的光谱仪,开展了Mn化合物和Th O2锕系化合物的实验。结果表明,该系统可以满足高能量分辨率实验的需求。

关键词：同步辐射高能量分辨谱仪 LabVIEW 运动控制数据采集

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时间分辨热化学原位XAFS方法

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化工进展 2024年第7期43卷 3747-3755页

作者：顾颂琦孙凡飞韦尧宋兴飞南兵李丽娜黄宇营中国科学院上海应用物理研究所上海201800 中国科学院上海高等研究院上海201204 中国科学院大学北京100049 沈阳化工大学特色资源化工与材料教育部重点实验室辽宁沈阳110142

为了利用X射线吸收精细结构(X-ray absorption fine structure,XAFS)谱学技术开展热化学反应动力学研究,在上海光源X射线吸收精细结构谱学线站(BL14W1)开展了时间分辨热化学原位XAFS方法的研究。采用自主研制的数据采集设备解决了时间分... 详细信息

为了利用X射线吸收精细结构(X-ray absorption fine structure,XAFS)谱学技术开展热化学反应动力学研究,在上海光源X射线吸收精细结构谱学线站(BL14W1)开展了时间分辨热化学原位XAFS方法的研究。采用自主研制的数据采集设备解决了时间分辨XAFS技术中不同类型信号同步触发和同步采集的问题,实现了数据间的精准匹配。在单色器转速为720"/s、数据采集设备采样率为2MS/s、数据长度为1200eV的条件下,获得了一个9.6s的Cu标样的数据谱,通过与常规XAFS数据和标准XAFS数据进行对比,结果表明本文得到的时间分辨XAFS实验系统具有良好的准确性、分辨率和信噪比。在此基础上,进一步结合线站自主研制的原位装置开展了时间分辨热化学原位XAFS方法,并利用高温常压原位装置开展了CuO还原为金属Cu的验证性实验。在230℃恒温氢气气氛下30min内观测到Cu吸收边能量逐渐向低能量处偏移,同时它位于8998eV的主峰强度逐渐减弱并且劈裂为双峰结构,出现明显的金属Cu的特征。实验结果表明此方法达到了捕获物质动态演化过程的预期目的,在拓展XAFS谱学实验平台的同时,为热化学反应的动力学过程研究提供了一种强大的实验手段。

关键词：时间分辨 X射线吸收精细结构原位装置热化学反应动力学

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