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C-H bond activation of propane on Ga_(2)O_(2)^(2+)in Ga/H-ZSM-5 and its mechanistic implications

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Chinese Journal of Catalysis 2024年第9期64卷 32-43页

作者： Zhaoqi Zhao Yunzhu Zhong Xiaoxia Chang bingjun xu Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains ***_(2)O_(2)^(2+)stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent *** we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+)species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+)species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al *** disparity in Ga_(2)O_(2)^(2+)species stems from their differing capacity in completing the catalytic *** results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+)species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+)species corresponding to GaHHW.

关键词： Propane dehydrogenation Ga2O22+ Activation of C-H bond Ga species

An Integrated Carbon Dioxide Capture and Methanation Process

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CCS Chemistry 2024年第5期6卷 1174-1183页

作者： Xiaochen Zhang Mengzhu Li Xingwu Liu Ang Li Yuchen Deng Mi Peng Yu Zhang Charlotte Vogt Matteo Monai Junxian Gao xuetao Qin Yao xu Qiaolin Yu Meng Wang Guofu Wang Zheng Jiang Xiaodong Han Casper Brady Wei-xue Li Wu Zhou Jin-xun Liu bingjun xu Bert M.Weckhuysen Ding Ma Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 China Academy of Aerospace Science and Innovation Beijing 100088 National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Beijing 101400 Beijing Key Laboratory of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing Inorganic Chemistry and Catalysis group Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials ScienceFaculty of ScienceUtrecht University3584 CG Utrecht State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001 Shanghai Synchrotron Radiation Facility Zhangjiang LadShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210 Center for Catalytic Science and Technology University of DelawareNewarkDelaware 19716 Key Laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefeiAnhui 230026 Hefei National Laboratory University of Science and Technology of ChinaHefei 230088 School of Physical Sciences CAS Key Laboratory of Vacuum PhysicsUniversity of Chinese Academy of SciencesBeijing 100049

Reducing the ever-growing level of CO_(2)in the atmosphere is critical for the sustainable development of human society in the context of global *** of the capture and upgrading of CO_(2)is,therefore,highly desirable since each process step is costly,both energetically and ***,we report a CO_(2)direct air capture(DAC)and fixation process that produces *** concentrations of CO_(2)(∼400 ppm)in the air are captured by an aqueous solution of sodium hydroxide to form *** carbonate is subsequently hydrogenated to methane,which is easily separated from the reaction system,catalyzed by TiO2-supported Ru in the aqueous phase with a selectivity of 99.9%among gas-phase *** concurrent regenerated hydroxide,in turn,increases the alkalinity of the aqueous solution for further CO_(2)capture,thereby enabling this one-ofits-kind continuous CO_(2)capture and methanation *** simulations demonstrate the energy feasibility of this CO_(2)DAC and methanation process,highlighting its promise for potential largescale applications.

关键词： CO_(2)capture and methanation process sodium hydroxide carbonate Ru/TiO_(2) catalytic mechanism CO_(2)activation and hydrogenation

Origin and effect of surface oxygen-containing species on electrochemical CO or CO_(2) reduction reactions

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Science China Chemistry 2023年第1期66卷 96-106页

作者： Xiaoxia Chang Ming He Qi Lu bingjun xu College of Chemistry and Molecular Engineering Peking UniversityBejing 100871China Department of Chemical Engineering Tsinghua UniversityBejing 100084China

Renewable-energy-powered electrochemical CO or CO_(2)reduction reactions(CO_(2)RR)provide one of the most promising strategies to upgrade CO_(2)to valuable *** the past decade,the existence and the mechanistic role of oxygen-containing species,such as(sub)surface oxide,hydroxide and oxyhydroxide species,at the electrode–electrolyte interface under reductive conditions have emerged as a topic of acute discussion within the CO_(2)RR ***-derived Cu attracted the most attention,while other surfaces,including Au,Ag and Sn,were also widely *** review identifies likely causes for contrasting results and views in the literature,summarizes possible oxygen sources for the interfacial oxygen-containing species at the CO_(2)RR conditions,and discusses potential roles these species could play in affecting the rate and product ***,perspectives on future efforts to reveal the identity and role of oxygen-containing species in the CO_(2)RR are presented.

关键词： electrochemical CO_(2)reduction surface oxygen-containing species copper-based catalysts

一种用于大型风电机组叶片自重载荷标定的弯矩解析方法研究

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电机与控制应用 2024年第7期51卷 74-83页

作者：吴蔚何中一徐秉俊中国质量认证中心上海分中心上海201206 上海中认尚科新能源技术有限公司上海201206 上海电器科学研究所(集团)有限公司上海200063

在大型风电机组的机械载荷测试中,叶片自重引起的摆振弯矩和挥舞弯矩的载荷标定精确度直接影响叶片和风轮的载荷测试效果。因此分析叶片自重在应变片测量位置的弯矩解析结果是叶片载荷标定的关键。首先,运用解析几何原理,提出了一种基... 详细信息

在大型风电机组的机械载荷测试中,叶片自重引起的摆振弯矩和挥舞弯矩的载荷标定精确度直接影响叶片和风轮的载荷测试效果。因此分析叶片自重在应变片测量位置的弯矩解析结果是叶片载荷标定的关键。首先,运用解析几何原理,提出了一种基于优选的三维坐标系和坐标变换的叶片自重弯矩解析方法。其次,为了消除主轴倾角对优选的三维坐标系的影响,提出了一种在优选的三维坐标系中调整叶片重力矢量方向的方法,并推导出了考虑各种影响因素下的弦摆振弯矩、弦挥舞弯矩的解析表达式。最后,在实际的叶片载荷测试项目中,应用两种标定分析方法进行对比,两种方法得到的叶片载荷测试结果具有很好的一致性和代表性。理论分析和试验结果验证了本文所提的叶片自重弯矩解析方法对叶片载荷标定的有效性和可行性。

关键词：风电机组机械载荷载荷标定解析几何弦摆振弯矩弦挥舞弯矩

Metal-organic layers induce in situ nano-structuring of Cu surface in electrocatalytic CO_(2)reduction

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Nano Research 2023年第4期16卷 4554-4561页

作者： Xinru He Jiawei Chen Yifei xu Yan Shen Yifan Zeng Jieyu Zhu bingjun xu Cheng Wang iChem State Key Laboratory of Physical Chemistry of Solid SurfacesCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China

Cu-based catalysts have attracted widespread attention for its capability in electrocatalytically reducing CO_(2)to a variety of *** modification of Cu has become an interesting method for tuning the catalytic ***,we use Zrbased metal-organic layers(MOLs)as the additive of the Cu surface,which enhanced the Faradaic efficiency of CH4 by two times as compared to the untreated polycrystalline Cu ***,the MOLs were found to induce in situ nano-structuring of the Cu foil surface within seconds in the electrolysis,as revealed by a combination of scanning electron microscopy(SEM),grazing incidence X-ray diffractometry(GIXRD),and linear sweep voltammetry(LSV)*** surface changes are responsible for the shift of product *** experiments suggest that negatively chargedμ3-O−on the Zr-cluster in the MOL might interact with CO-covered Cu surface and induce roughing and *** work reveals a potential role of additive on Cu to induce surface nano-structuring that tunes catalytic activity and selectivity.

关键词： CO_(2)reduction CO_(2)methanation metal-organic layers Cu foil surface nano-structuring

Oxidative co-dehydrogenation of ethane and propane over h-BN as an effective means for C-H bond activation and mechanistic investigations

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Chinese Journal of Catalysis 2022年第8期43卷 2173-2182页

作者： Hao Tian bingjun xu Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Hexagonal boron nitride(h-BN)is a highly selective catalyst for oxidative dehydrogenation of light alkanes to produce the corresponding *** intense recent research effort,many aspects of the reaction mechanism,such as the observed supra-linear reaction order of alkanes,remain *** this work,we show that the introduction of a low concentration of propane in the feed of ethane oxidative dehydrogenation is able to enhance the C_(2)H_(6) conversion by 47%,indicating a shared reaction intermediate in the activation of ethane and *** higher activity of propane makes it the dominant radical generator in the oxidative co-dehydrogenation of ethane and propane(ODEP).This unique feature of the ODEP renders propane an effective probe molecule to deconvolute the two roles of alkanes in the dehydrogenation chemistry,i.e.,radical generator and *** studies indicate that both the radical generation and the dehydrogenation pathways exhibit a first order kinetics toward the alkane partial pressure,leading to the observed second order kinetics of the overall oxidative dehydrogenation *** the steady-state approximation,a radical chain reaction mechanism capable of rationalizing observed reaction behaviors is proposed based on these *** work demonstrates the potential of ODEP as a strategy of both activating light alkanes in oxidative dehydrogenation on BN and mechanistic investigations.

关键词： Hexagonal boron nitride Oxidative dehydrogenation Radical chain reaction Reaction order C-H activation

2011—2022年浙江省衢州市人间布鲁氏菌病流行特征及菌型分布

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中华卫生杀虫药械 2024年第4期30卷 369-373页

作者：邓小雁郑水萍钟建跃潘婉徐冰俊衢州市疾病预防控制中心浙江衢州324000

目的分析2011—2022年衢州市人间布鲁氏菌病(简称“布病”)流行病学特征及菌型分布,为制定衢州市布病防控措施提供依据。方法布病病例资料来自传染病网络直报系统,人口学资料来自《衢州市统计年鉴》。对衢州市2011—2022年布病报告病... 详细信息

目的分析2011—2022年衢州市人间布鲁氏菌病(简称“布病”)流行病学特征及菌型分布,为制定衢州市布病防控措施提供依据。方法布病病例资料来自传染病网络直报系统,人口学资料来自《衢州市统计年鉴》。对衢州市2011—2022年布病报告病例的流行病学特征进行统计学描述与分析。结果 2011—2022年衢州市布病报告总数为89例,年均发病率为0.290/10万,2021年发病率达高峰,为0.662/10万;全年均有病例报告,发病集中在3~8月,占病例报告总数的77.528%(69例)。全市仅开化县无病例报告,报告病例数占比最高为衢江区,占病例报告总数的31.461%(28例)。男性报告病例总数为64例,女性报告病例总数为25例,男女性别比为2.560∶1。发病人群主要集中于50~59岁年龄组,报告病例数为41例,占总报告病例数的46.067%;农民报告病例数最多,共69例,占总报告病例数的77.528%。所有病例中血培养共分离出菌株12株,经鉴定分型均为羊种型布氏菌属,羊种Ⅰ型和Ⅲ型各为6例。结论衢州市人间布病疫情总体处于散发、局部爆发并存的低流行水平。防控重点人群是从事羊养殖、羊屠宰行业的农村青壮年男性人员,但近几年随着餐饮业盛行烤羊肉及羊肉串,餐饮服务人员发病数占一定比例。建议加强联防联控,市农业农村局加强源头管控,要求养殖场及屠宰场尽量从正规渠道引进检疫合格的牲畜,同时加强落地抽检,及时发现及处置传染病畜。卫生健康部门加强重点人群健康宣教和主动监测工作,提高群众知信行合一能力,做到早预防、早发现、早治疗,以进一步降低人间布病对衢州地区群众身体健康造成的不良影响。

关键词：布鲁氏菌病流行病学特征菌型分布

Evolution of China's Accessibility Standard System and International Experience

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China City Planning Review 2021年第3期30卷 37-44页

作者： xu bingjun Shao Lei Li Min(译) Liu Jiayan(校) School of Architecture Tsinghua UniversityBeijingP.R.China Institute for Accessibility Development Tsinghua UniversityBeijingP.R.China 不详

This paper summarizes the evolution of China’s accessibility standard system and its driving forces since the reform and opening-up was introduced in 1978,divides it into several stages based on social and economic development,and further analyzes its development trend in the context of standardization ***,it critically reviews the characteristics of China’s current accessibility standard system and problems encountered during the implementation ***,it proposes suggestions for the development of China’s accessibility standard system in the new era by drawing on domestic and international experience.

关键词： the accessible environment construction standard system legislation on accessibility universal accessibility participation of persons with disabilities

PdFe金属间化合物表面可逆氧化还原过程对CO_(2)甲烷化反应的促进和稳定作用

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物理化学学报 2021年第5期37卷 14-15页

作者：徐冰君北京大学化学与分子工程学院北京100871

CO_(2)加氢技术可以实现氧的回收,这为密闭空间人的呼吸用氧问题提供了解决方案,因此在某些特殊场景具有重要的战略意义,例如通过CO_(2)甲烷化维持空间站的生命保障系统1,2。在空间站和宇宙飞船中,宇航员呼吸所需的O2来自电解水,这个过... 详细信息

CO_(2)加氢技术可以实现氧的回收,这为密闭空间人的呼吸用氧问题提供了解决方案,因此在某些特殊场景具有重要的战略意义,例如通过CO_(2)甲烷化维持空间站的生命保障系统1,2。在空间站和宇宙飞船中,宇航员呼吸所需的O2来自电解水,这个过程也伴随着H2的产生。由于空间站和宇宙飞船的载荷有限,无法携带大量的水,这就限制了所能提供O2量,无法维持长时间的太空航行。

关键词：生命保障系统宇宙飞船空间站氧化还原过程密闭空间金属间化合物电解水甲烷化