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Identifying the roles of Ce^(3+)-OH and Ce-H in the reverse water-gas shift reaction over highly active Ni-doped CeO_(2) catalyst

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Nano Research 2022年第7期15卷 5831-5841页

作者： Haidong Shen Yujuan Dong Shaowei Yang Yuan He Qimeng Wang Yueling Cao Wenbin Wang Tianshuai Wang Qiuyu Zhang Hepeng Zhang Xi’an Key Laboratory of Functional Organic Porous Materials School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710129China Research&Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518057China

Nickel-CeO_(2)-based materials are commonly used for the thermal catalytic hydrogenation of CO_(2).However,high Ni loadings and low CO selectivity restrict their use in the reverse water–gas shift(RWGS)***,we demonstrate a highly active,robust,and low-Ni-doped(1.1 wt.%)CeO_(2) catalyst(1.0-Ni-CeO_(2)).The Ni-based-mass-specific CO formation rate reaches up to 1,542 mmol·gNi^(−1)·h^(−1) with 100%CO selectivity at 300°C for 100 h,among the best values reported in the *** functional theory(DFT)and diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)results reveal that the enhanced catalytic activity is attributed to the abundant Ce–H species,while the high selectivity results from low CO *** importantly,a new reaction mechanism is proposed,which involves the reduction of bicarbonate to generate formate intermediate and CO by the H−released from Ce–H *** new findings in this work will benefit the design of economic,efficient,and robust catalysts for low-temperature RWGS reactions.

关键词： CO_(2)hydrogenation Ni-doped CeO_(2) reverse water-gas shift(RWGS)reaction cerium hydride mechanism investigation

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Effect of Ni particle size on the production of renewable methane from CO_(2) over Ni/CeO_(2) catalyst

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Journal of Energy Chemistry 2021年第10期30卷 602-611,I0015页

作者： Lili Lin Clifford A.Gerlak Chang Liu Jordi Llorca Siyu Yao Ning Rui Feng Zhang Zongyuan Liu Sen Zhang Kaixi Deng Christopher B.Murray José A.Rodriguez Sanjaya D.Senanayake Chemistry Division Brookhaven National LaboratoryUptonNY 11973USA Institute of Industrial Catalysis State Key Laboratory of Green Chemistry Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014ZhejiangChina Department of Chemistry University of VirginiaCharlottesvilleVA 22904USA Institute of Energy Technologies Department of Chemical Engineering and Barcelona Research Center in Multiscale Science and EngineeringUniversitat Politècnica de CatalunyaEEBEEduard Maristany 10-1408019 BarcelonaSpain Zhejiang University Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Chemistry Department State University of New YorkStony BrookNYUSA Departments of Chemistry and Materials Science&Engineering University of Pennsylvania231 South 34th Street394PhiladelphiaPA 19104USA

Production of’renewable Methane’has attracted renewed research interest as a fundamental probe reaction and process for CO_(2)utilization through potential use in Cl fuel production and even for future space exploration ***_(2)methanation is a structure sensitive reaction on Ni/CeO_(2)*** precisely elucidate the size effect of the Ni metal center on the CO_(2)methanation performance,we prepared2%Ni/CeO_(2)catalysts with pre-synthesized uniform Ni particles(2,4 and 8 nm)on a high surface area CeO_(2)*** electron microscopy(TEM)and ambient pressure X-ray photo spectroscopy(AP-XPS)characterization have confirmed that the catalyst structure and chemical state was uniform and stable under reaction *** 8 nm sized catalyst showed superior methanation selectivity over the 4 and 2 nm counterparts,and the methanation activity in term of TOF is 10 times and 70 times higher than for the 4 and 2 nm counterparts,*** DRIFTS studies revealed that the larger Ni(8 nm particles)over CeO_(2)efficiently facilitated the hydrogenation of the surface formate intermediates,which is proposed as the rate determining step accounting for the excellent CO_(2)methanation performance.

关键词： CO_(2)methanation Particle size effect Ni/CeO_(2) In situ DRIFTS mechanism investigation

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Coal and gas outburst mechanism of the “Three Soft” coal seam in western Henan

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Mining Science and Technology 2010年第5期20卷 712-717页

作者： LEI DongJi LI Chengwu ZHANG Zimin ZHANG Yugui Faculty of Resources & Safety Engineering China University of Mining & Technology Beijing 100083 China School of Safety Science and Engineering Henan Polytechnic University Jiaozuo 454003 China

Based on the particularities of gas outbursts,i.e.,low gas bearing capacity and low gas pressure in the "Three Soft" coal seam in western Henan,we applied the theories of plate tectonics and regional structural evolution to investigate the mechanism of this seam and its impact on the coal seam gas *** investigation revealed that coal and gas outbursts are distributed in a strip in a NW direction,with a number of high-penetration mines scattered towards the south side and low-gas mines largely located on the north *** analyzed the statistics of 38 gas explosions and the rock-coal sturdiness number coefficient f of 167 sampling sites in the region and found the gas outburst mechanism that features a "low indicator outburst phenomenon".The mechanism is characterized by structural coal as its core,a low gas bearing capacity,low gas pressure and sturdiness coefficient f mostly less than *** research results provide a theoretical foundation for effective control of gas disasters.

关键词： coal and gas outburst mechanism investigation threshold sliding structure

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"Win-Win"Scenario of High Energy Density and Long Cycling Life in a Novel Na_(3.9)MnCr_(0.9)Zr_(0.1)(PO_(4))_(3)Cathode

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Energy & Environmental Materials 2024年第1期7卷 83-90页

作者： Yao Wang Yukun Liu Pingge He Junteng Jin Xudong Zhao Qiuyu Shen Jie Li Xuanhui Qu Yongchang Liu Lifang Jiao Beijing Advanced Innovation Center for Materials Genome Engineering State Key Laboratory for Advanced Metals and MaterialsInstitute for Advanced Materials and TechnologyUniversity of Science and Technology BeijingBeijing 10083China Department of Chemistry and Biochemistry University of California1156 High StreetSanta CruzCA 95064USA Tianjin Key Laboratory for Photoelectric Materials and Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The development of high-energy and long-lifespan NASICON-type cathode materials for sodium-ion batteries has always been a research hotspot but a daunting *** Na_(4)MnCr(PO_(4))_(3)has emerged as one of the most promising high-energy-density cathode materials owing to its three-electron reactions,it still suffers from serious structural distortion upon repetitive charge/discharge processes caused by the Jahn-Teller active Mn^(3+).Herein,the selective substitution of Cr by Zr in Na_(4)MnCr(PO_(4))_(3)was explored to enhance the structural stability,due to the pinning effect of Zr ions and the≈2.9-electron reactions,as-prepared Na_(3.9)MnCr_(0.9)Zr_(0.1)(PO_(4))_(3)/C delivers a high capacity retention of 85.94%over 500 cycles at 5 C and an ultrahigh capacity of 156.4 mAh g^(-1)at 0.1 C,enabling the stable energy output as high as 555.2 Wh kg^(-1).Moreover,during the whole charge/discharge process,a small volume change of only 6.7%was verified by in situ X-ray diffraction,and the reversible reactions of Cr^(3+)/Cr^(4+),Mn^(3+)/Mn^(4+),and Mn^(2+)/Mn^(3+)redox couples were identified via ex situ X-ray photoelectron spectroscopy *** intermittent titration technique tests and density functional theory calculations further demonstrated the fast reaction kinetics of the Na_(3.9)MnCr_(0.9)Zr_(0.1)(PO_(4))_(3)/C *** work offers new opportunities for designing high-energy and high-stability NASICON cathodes by ion doping.

关键词： high energy density mechanism investigation NASICON-type cathodes sodium-ion batteries structure modification

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