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Journal of Energy Chemistry 2019年第6期28卷 31-36页

作者： Fei Huang Zhimin Jia jiangyong diao Hua Yuan Dangsheng Su Hongyang Liu Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina School of Materials Science and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina College of Chemistry Chongqing Normal UniversityChongqing 401331China

We report a nanocarbon material with nanodiamond(ND) core and graphene shell(ND@G) as a support for Pd nanocatalysts. The designed catalyst performed good selectivity of styrene(85.2%) at full conversion of phenylacetylene and superior stability under mild conditions. Supported Pd catalysts are characterized by means of high resolution transmission electron microscopy(HRTEM), Raman, X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS) and H2 temperature-programmed reduction(H2-TPR).The results clearly show that formation of the strong metal-support interaction(SMSI) between Pd nanoclusters and the defective graphene shell helpfully modifies the selectivity and stability of the Pd-based catalysts.

关键词： Selective hydrogenation Palladium nano clusters Nanocarbon support Liquid-phase hydrogenation

Fabrication of three dimensional SiC@C hybrid for efficient direct dehydrogenation of ethylbenzene to styrene

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Journal of Materials Science & Technology 2022年第8期103卷 209-214页

作者： Jiashun Wang Linlin Wang jiangyong diao Xi Xie Guoming Lin Qing Jia Hongyang Liu Guoxin Sui Shi-changxu Innovation Center for Advanced Materials Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaHefei 230026China Department of Chemistry Northeastern UniversityShenyang 110819China

Synthesis of hybrid carbon materials with core-shell structure and robust catalytic performance is of great research interest,and remains a great challenge in catalytic dehydrogenation of hydrocarbons *** this paper,few-layer sp^(2) carbon decorated SiC nanocrystals with core-shell structure(SiC@C)were fabricated through a dual-confined magnesiothermic method by employing glucose and SiO_(2) as *** SiC@C nanocrystals were further crosslinked to be a three dimensional(3D)mesoporous hybrid by the in situ generated carbon as binders and exhibiting a 410.30 m^(2) g^(−1) large surface *** as-prepared SiC@C hybrid materials as metal-free catalysts were evaluated in the steam-free direct dehydrogenation of ethylbenzene to *** from the abundant surface carbonyl groups on the graphite carbon layers,the optimized yield rate of styrene normalized by carbon mass was as high as 11.58 mmol g^(−1) carbon h^(−1),nearly 4 times that of *** the low cost and excellent catalytic activity,the hybrid 3D SiC@C material may be a promising candidate for direct dehydrogenation of hydrocarbons.

关键词： Silicon carbide Carbon material Core-shell structure Heterogeneous catalysis Direct dehydrogenation Ethylbenzene

Fully-exposed Pt clusters stabilized on Sn-decorated nanodiamond/graphene hybrid support for efficient ethylbenzene direct dehydrogenation

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Nano Research 2022年第12期15卷 10029-10036页

作者： Linlin Wang Xuetao Qin Ting Sun Xiangbin Cai Mi Peng Zhimin Jia Xiaowen Chen Ning Wang jiangyong diao Hongyang Liu Ding Ma Department of Chemistry Northeastern UniversityShenyang110819China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang110016China Beijing National Laboratory for Molecular Engineering College of Chemistry and Molecular Engineering and College of EngineeringBIC-ESATPeking UniversityBeijing100871China Department of Physics Hong Kong University of Science and TechnologyKowloonHong Kong999077China School of Materials Science and Engineering University of Science and Technology of ChinaHefei230026China

The pursuit of energy conservation and environmental protection has always been a hot topic in the catalytic fields,which is inseparable from the rational designing of efficient catalysts and an in-depth understanding of the catalytic reaction *** this work,fully-exposed Pt clusters were fabricated on the atomically dispersed Sn decorated nanodiamond/graphene(Sn-ND@G)hybrid support and employed for direct dehydrogenation(DDH)of ethylbenzene(EB)to styrene(ST).The detailed structural characterizations revealed the fully-exposed Pt clusters were stabilized on Sn-ND@G,assisted by the spatial separation of atomically dispersed Sn *** as-prepared Pt/Sn-ND@G catalyst showed enhanced ST yield(136.2 molEB·molpt-1·h-1 EB conversion rate and 99.7%ST selectivity)and robust long-term stability at 500℃for the EB DDH reaction,compared with the traditional ND@G supported Pt nanoparticle catalyst(Pt/ND@G).The ST prefers to desorb from the fully-exposed Pt clusters,resulting in the enhanced DDH catalytic performance of the Pt/Sn-ND@G *** present work paves a new way for designing highly dispersed and stable supported metal catalysts for DDH reactions.

关键词： Pt cluster ethylbenzene dehydrogenation fully-exposed catalyst heterogeneous catalysis

Boron nitride for enhanced oxidative dehydrogenation of ethylbenzene

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Journal of Energy Chemistry 2021年第6期30卷 477-484,I0012页

作者： Rui Han jiangyong diao Sonu Kumar Andrey Lyalin Tetsuya Taketsugu Gilberto Casillas Christopher Richardson Feng Liu Chang Won Yoon Hongyang Liu Xudong Sun Zhenguo Huang Key Laboratory for Anisotropy and Texture of Materials(Ministry of Education) Northeastern UniversityShenyang 110819LiaoningChina School of Civil and Environmental Engineering University of Technology SydneyUltimoNew South Wales 2007Australia Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina Institute for Chemical Reaction Design and Discovery(WPI-ICReDD) Hokkaido UniversitySapporo 001-0021Japan Center for Green Research on Energy and Environmental Materials National Institute for Materials Science(NIMS)Tsukuba 305-0044Japan Department of Chemistry Faculty of ScienceHokkaido UniversitySapporo 060-0810Japan Electron Microscopy Centre University of WollongongNew South Wales 2500Australia Molecular Horizons and School of Chemistry and Molecular Bioscience Faculty of ScienceMedicine and HealthUniversity of WollongongNew South Wales 2522Australia Center for Hydrogen and Fuel Cell Research Korea Institute of Science and TechnologySeoul 02792Republic of Korea

It is demonstrated experimentally and confirmed theoretically that highly defective boron nitride showed outstanding performance for oxidative dehydrogenation of *** catalyst is derived from carbon-doped hexagonal boron nitride nanosheets synthesized via a two-step reaction when participating the oxidative dehydrogenation *** first step yields a polymeric precursor with the atomic positions of B,C,N relatively constrained,which is conducive for the formation of carbon atomic clusters uniformly dispersed throughout the BN *** the oxidative dehydrogenation of ethylbenzene to styrene,the nanoscale carbon clusters are removed and highly defective boron nitride(D-BN)is obtained,exposing boron-rich zigzag edges of BN that act as the catalytic *** catalytic performance of D-BN is therefore remarkably better than un-doped *** results indicate that dispersed C-doping in h-BN is highly effective in terms of defect formation and resultant enhanced activity in oxidative dehydrogenation reactions.

关键词： Boron nitride Dehydrogenation Ethylbenzene Carbon-doping Heterogeneous catalysis

A MoS_2 nanocatalyst with surface-enriched active sites for the heterogeneous transfer hydrogenation of nitroarenes

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Chinese Journal of Catalysis 2018年第1期39卷 79-87页

作者： Jia Wang Yajie Zhang jiangyong diao Jiayun Zhang Hongyang Liu Dangsheng Su Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Shenyang 110016 Liaoning China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou 730000Gansu China School of Materials Science and Engineering University of Science and Technology of China Shenyang 110016 Liaoning China Energy Research Resources Division Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Liaoning China

A highly efficient and reusable plane‐curved and interlayer‐expanded MoS2nanocatalyst with increased exposure of active sites was *** catalyst was used for the heterogeneous hydrogen transfer reaction of nitroarenes with hydrazine monohydrate as a reductant under mild reaction conditions without pressure and base,which was different from other hydrogen transfer systems that require the presence of a base(e.g.,propan‐2‐ol/KOH).The sandwiching of carbon between the MoS2nanosheets increased the distance between the layers of MoS2and exposed more Mo sites,resulting in superior catalytic performance compared with that of bulk *** active hydrogen(H*)generated from N2H4could directly transfer to the–NO2groups of nitrobenzene to form aniline followed by N2emission,which was confirmed by detecting the gas emission with mass spectrometry during the decomposition of hydrazine or the co‐existence of nitrobenzene and hydrazine.?2018,Dalian Institute of Chemical Physics,Chinese Academy of *** by Elsevier *** rights reserved.

关键词： Molybdenum disulfide Interlayer expansion Hydrogen transfer reaction Nitrobenzene reduction Alkali‐free

C包覆Ni磁性载体负载Pt催化硝基苯加氢性能

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金属学报 2024年第8期60卷 1141-1149页

作者：武逸司阳黄彦民刁江勇孟繁敬刘增刘洪阳中国科学院金属研究所沈阳材料科学国家研究中心沈阳110016 沧州大化股份有限公司河北省改性异氰酸酯技术创新中心沧州061000

苯胺是一种重要的基础化工原料,在医药、染料、橡胶等领域被广泛应用。以硝基苯为原料通过液相催化加氢制备苯胺是目前主要工业生产方法之一,然而,如何从液相加氢反应体系中将催化剂高效分离和回收仍然是该领域的一个重要挑战。本工作... 详细信息

苯胺是一种重要的基础化工原料,在医药、染料、橡胶等领域被广泛应用。以硝基苯为原料通过液相催化加氢制备苯胺是目前主要工业生产方法之一,然而,如何从液相加氢反应体系中将催化剂高效分离和回收仍然是该领域的一个重要挑战。本工作开发了一种具有磁可分的C包覆Ni磁性载体负载Pt金属催化剂,用于高效催化硝基苯加氢制苯胺。以乙二胺四乙酸和Ni(OH)_(2)为原料成功合成了N掺杂石墨烯包覆Ni纳米颗粒磁性载体(Ni@NG),采用沉积-沉淀法制备Ni@NG负载Pt金属催化剂(Pt/Ni@NG),通过Raman光谱、TEM、XRD和XPS对制备的Pt/Ni@NG催化剂进行结构表征。结果表明,这种Ni@NG载体具有典型的核壳结构(纳米Ni颗粒为核,石墨烯为壳层)。XPS结果表明Ni@NG载体表面N掺杂石墨烯壳含有3.64%N (原子分数)。当Pt负载量(质量分数)从0.1%增加到0.5%时,Pt在石墨烯壳层表面的分散状态经历了单原子、团簇、颗粒的转变过程。当Pt负载量为0.3%时,以Pt团簇形式分散为主的Pt/Ni@NG催化硝基苯加氢显示出最高的活性,在反应压力为1 MPa和反应温度为30℃时,硝基苯加氢的周转频率为27239.2 h^(-1),硝基苯在60 min内完全转化为苯胺。此外,由于Pt/Ni@NG催化剂具有优异的液相磁可分性能,催化剂经5 cyc使用后加氢活性未明显降低。

关键词：核壳结构硝基苯加氢磁可分载体 N掺杂C材料

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论中日钓鱼岛主权争议问题

太平洋学报 2011年第3期19卷 72-86页

作者：刘江永清华大学北京100084

钓鱼岛自古以来是中国的固有领土。中日之间的钓鱼岛问题,是甲午战争遗留下来的、与"二战"后美国横加干预密切相关的岛屿及相关海域的主权争议问题;是涉及到民族感情、地缘政治、资源能源、台湾问题等容易影响中日关系全局的局部敏感问... 详细信息

钓鱼岛自古以来是中国的固有领土。中日之间的钓鱼岛问题,是甲午战争遗留下来的、与"二战"后美国横加干预密切相关的岛屿及相关海域的主权争议问题;是涉及到民族感情、地缘政治、资源能源、台湾问题等容易影响中日关系全局的局部敏感问题,牵一发而动全身。要妥善处理中日之间的敏感问题,促使中日关系健康发展,首先需了解钓鱼岛主权归属问题历史真相的来龙去脉、正确的国际法解释,并对容易引起误解的若干问题加以必要的说明与澄清。

关键词：钓鱼岛主权争议中日关系国际法