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Heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation

Journal of Energy Chemistry 2024年第6期93卷 419-428,I0011页

作者： Qi Zhang quanguo jiang Xiang Yang Chi Zhang Jian Zhang Lu Yang Haiyan He Guobing Ying Huajie Huang College of Materials Science and Engineering Hohai UniversityNanjing 210098JiangsuChina New Energy Technology Engineering Lab of jiangsu Province College of ScienceNanjing University of Posts&Telecommunications(NUPT)Nanjing 210023JiangsuChina School of Materials Science and Engineering Southeast UniversityNanjing 211100JiangsuChina

Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative ***,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly *** unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic *** a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading *** functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO *** work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.

关键词： Rhodium nanosheet Ti_(3)C_(2)T_(x)MXene Heterointerface Electrocatalyst Fuel cell

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Ultra-high-temperature application of MXene: Stabilization of 2D Ti_(3)C_(2)T_(x) for cross-scale strengthening and toughening of 3D TiC

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Journal of Advanced Ceramics 2024年第1期13卷 1-10页

作者： Lu Liu Guobing Ying quanguo jiang Dong Wen Peng Wang Meng Wu Ziying Ji Yongting Zheng Xiang Wang Department of Materials Science and Engineering College of Mechanics and MaterialsHohai UniversityNanjing 211100China Key Laboratory of Superlight Materials&Surface Technology Ministry of EducationHarbin Engineering UniversityHarbin 150001China Shenzhen Key Laboratory for Advanced Materials School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China Center for Composite Materials and Structures Harbin Institute of TechnologyHarbin 150001China

Transition metal carbide/nitride cores within MXenes make them considerably useful for ultra-high-temperature ***,extensive research on Ti_(3)C_(2)T_(x) MXene has revealed its tendency to undergo a phase transition to TiCy at temperatures above 800℃due to high activity of a superficial Ti atomic ***,spark plasma sintering of Ti_(3)C_(2)T_(x) and TiC is performed to prevent the Ti_(3)C_(2)T_(x) phase transition at temperatures up to 1900℃through the fabrication of composites at a pressure of 50 *** a focused ion beam scanning electron microscope to separate layered substances in the composites and examining selected area diffraction spots in a transmission electron microscope enabled identification of non-phase-transitioned ***-principles calculations based on density functional theory indicated the formation of strong chemical bonding interfaces between Ti_(3)C_(2)T_(x) and TiC,which imposed a stability constraint on the Ti atomic layer at the Ti_(3)C_(2)T_(x) *** performance tests,such as three-point bending and fracture toughness analysis,demonstrated that the addition of Ti_(3)C_(2)T_(x) can effectively improve the cross-scale strengthening and toughening of the TiC matrix,providing a new path for designing and developing two-dimensional(2D)carbides cross-scale-enhanced three-dimensional(3D)carbides with the same elements relying on a wide variety of MXenes.

关键词： MXene ultra-high-temperature phase stability interface bonding cross-scale strengthening and toughening structural ceramic composites

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Constructing 3D interweaved MXene/graphitic carbon nitride nanosheets/graphene nanoarchitectures for promoted electrocatalytic hydrogen evolution

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Journal of Energy Chemistry 2022年第4期31卷 483-491页

作者： Haiyan He Yuxian Chen Cuizhen Yang Lu Yang quanguo jiang Huajie Huang College of Mechanics and Materials Hohai UniversityNanjing 210098JiangsuChina Institute of Ocean and Offshore Engineering Hohai UniversityNantong 226300JiangsuChina

The technique of electrocatalytic hydrogen evolution reaction (HER) represents a development trend of clean energy generation and conversion,while the electrode catalysts are bound to be the core unit in the electrochemical HER ***,we demonstrate a bottom-up approach to the construction of three-dimensional (3D) interconnected ternary nanoarchitecture originated from Ti_(3)C_(2)T_(x)MXene,graphitic carbon nitride nanosheets and graphene (MX/CN/RGO) through a convenient co-assembly *** virtue of the 3D porous frameworks with ultrathin walls,large specific surface areas,optimized electronic structures,high electric conductivity,the resulting MX/CN/RGO nanoarchitecture expresses an exceptional HER performance with a low onset potential of only 38 m V,a small Tafel slop of 76 m V dec^(-1) as well as long lifespan,all of which are more competitive than those of the bare Ti_(3)C_(2)T_(x),g-C_(3)N_(4),graphene as well as binary MX/RGO and CN/RGO *** simulations further verify that the ternary MX/CN/RGO nanoarchitecture with ameliorative band structure is able to facilitate the electron transport and meanwhile offer multistage catalytically active sites,thereby guaranteeing rapid HER kinetics during the electrocatalytic process.

关键词： MXene Carbon nitride Graphene Electrocatalysts Hydrogen evolution

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Strain boosts CO oxidation on Ni single-atom-catalyst supported by defective graphene

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Chinese Chemical Letters 2023年第2期34卷 295-300页

作者： quanguo jiang Yushuai Qian Yuqing Liu Min Huang Zhimin Ao College of Mechanics and Materials Hohai UniversityNanjing 210098China Guangzhou Key Laboratory Environmental Catalysis and Pollution Control Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlInstitute of Environmental Health and Pollution ControlSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

In order to realize the sulfur and water resistance and facilitate the CO oxidation reactions,the effects of strain on the adsorption of CO,O_(2),SO_(2)and H_(2)O molecules on Ni single-atom-catalyst supported by single-carbon-vacancy graphene(Ni-SG) have been studied based on first principles *** shows that the compressive strain increases the adsorption energies of all above mentioned molecules on Ni-SG,where SO_(2)is adsorbed more strongly on Ni-SG than ***,in the presence of tensile strain,the adsorption energies decreases significantly when the molecules(O_(2)and SO_(2)) obtain electrons from NiSG,while the adsorption energies just slightly decrease when the molecules(CO and H_(2)O) lose electrons to Ni-SG,which finally achieves the preferential adsorption of CO and O_(2)molecules on Ni-SG by tensile *** addition,with tensile strain increasing to 10%,the rate-limited energy barrier along Eley-Rideal(ER) path monotonically increases from 0.77 eV to 0.98 eV,while the rate-limited energy barrier along Langmuir-Hinshelwood(LH) path monotonically decreases from 0.54 eV to 0.44 eV,indicating that the tensile strain can facilitate the LH mechanism while imped the ER mechanism on *** Hirshfeld charge and orbital levels of O_(2)and CO molecules are modulated by the tensile strain,which plays an important role for the decreasing of energy barriers for CO ***,the tensile strain can enhance the sulfur and water resistance of Ni-SG,as well as boost the CO oxidation reactions.

关键词： Strain effect Ni single-atom-catalyst Preferential adsorption CO oxidation First principles calculations

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Density functional theory investigation on selective adsorption of VOCs on borophene

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Chinese Chemical Letters 2021年第9期32卷 2803-2806页

作者： Wenlang Li quanguo jiang Didi Li Zhimin Ao Taicheng Ana Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control Guangzhou Key Laboratory of Environmental Catalysis and Pollution ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China College of Mechanics and Materials Hohai UniversityNanjing 210098China

In the field of volatile organic compounds(VOCs)pollution control,adsorption is one of the major control methods,and effective adsorbents are desired in this *** this work,the density functional theory(DFT)calculations are employed to investigate the adsorption of typical VOCs molecules on the two-dimensional material *** results demonstrate that both structure ofχBorophene;2D material;Volatile organic compounds(VOCs);Selective adsorption;Electronic structure andβ12 borophene can chemically adsorb ethylene and formaldehyde with forming chemical bonds and releasing large ***,other VOCs,including ethane,methanol,formic acid,methyl chloride,benzene and toluene,are physically adsorbed with weak *** analysis of density of states(DOS)reveals that the chemical adsorption changes the conductivity of borophenes,while the physical adsorption has no distinct effect on the ***,bothχ^(3)andβ_(12) borophene are appropriate adsorbents for selective adsorption of ethylene and formaldehyde,and they also have potential in gas sensor applications due to the obvious conductivity change during the adsorption.

关键词： Borophene 2D material Volatile organic compounds(VOCs) Selective adsorption Electronic structure

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Controllable synthesis of grain boundary-enriched Pt nanoworms decorated on graphitic carbon nanosheets for ultrahigh methanol oxidation catalytic activity

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Journal of Energy Chemistry 2021年第6期30卷 601-609,I0014页

作者： Huajie Huang Yujie Wei Ying Yang Minmin Yan Haiyan He quanguo jiang Xiaofei Yang Jixin Zhu College of Mechanics and Materials Hohai UniversityNanjing 210098JiangsuChina jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of ScienceNanjing Forestry UniversityNanjing 210037JiangsuChina Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing 211816JiangsuChina

Although one-dimensional Pt nanocrystals have long been regarded as ideal electrode catalysts for fuel cells,the synthetic techniques commonly involve the use of various complicated templates or surfactants,which have largely hampered their large-scale industrial ***,we present a convenient and cost-effective approach to the stereoassembly of quasi-one-dimensional grain boundary-enriched Pt nanoworms on nitrogen-doped low-defect graphitic carbon nanosheets(Pt NWs/NL-CNS).Benefiting from its numerous catalytically active grain boundaries as well as optimized electronic structure,the as-derived Pt NWs/NL-CNS catalyst possesses exceptionally good electrocatalytic properties for methanol oxidation,including an ultrahigh mass activity of 1949.5 mA mg^(-1), reliable long-term durability,and strong poison tolerance,affording one of the most active Pt-based electrocatalysts for methanol oxidation *** functional theory calculation further reveals that the formation of worm-shape Pt morphology is attributed to the modified electronic structure as well as controllable defect density of the carbon matrix,which could also weaken the adsorption ability of Pt towards CO molecule and meanwhile synergistically promotes the catalytic reaction kinetics.

关键词： Platinum nanoworm Nitrogen doping Low defect Carbon nanosheet Methanol oxidation

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传感器放置位置对花岗岩岩爆声发射频谱特征的影响

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岩石力学与工程学报 2018年第A2期37卷 3968-3978页

作者：贾雪娜姜全果何满潮宫伟力山东交通学院交通土建工程学院山东济南250357 山东省地质测绘院山东济南250002 中国矿业大学(北京)深部岩土力学与地下工程国家重点实验室北京100083

为了验证岩爆试验过程中声发射传感器安装位置对采集的声发射信号的影响,以期通过声发射信号的分析得到正确的岩爆信息,采集花岗岩试样,开展传感器直接安装在岩样上和安装在岩样夹持垫块上的真三轴卸载岩爆试验研究。基于应变岩爆试验... 详细信息

为了验证岩爆试验过程中声发射传感器安装位置对采集的声发射信号的影响,以期通过声发射信号的分析得到正确的岩爆信息,采集花岗岩试样,开展传感器直接安装在岩样上和安装在岩样夹持垫块上的真三轴卸载岩爆试验研究。基于应变岩爆试验加载路径,将应变岩爆试验过程分为3个典型阶段,从3个阶段中选取每例应变岩爆试验中声发射信号的6个典型关键区段进行分析。结果表明:岩样夹持垫块相当于一个高通滤波器,即传感器在夹持垫块上的声发射信号只有高频带信号,不能反映岩样的破坏阶段形成的低频振动信息;而传感器直接在岩样上的声发射信号同时具有高频与低频带的信息,能够全面反映岩样加载过程中微裂纹扩展、汇合直至宏观破坏的全频段信息;同时,垫块对声发射信号的辐值具有衰减作用,即降低了信噪比,有可能使得一些主辐值信息难以识别。

关键词：岩石力学声发射传感器信号采集滤波器信噪比

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单原子催化剂Ti/Ti3C2O2催化氧化甲醛的密度泛函理论研究

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Chinese Journal of Catalysis 2020年第10期41卷 1633-1644页

作者：周君慧刘冠兰姜全国赵伟娜敖志敏安太成广东工业大学环境健康与污染控制研究院环境科学与工程学院广东省环境催化与健康风险控制重点实验室广东广州510006 河海大学力学与材料学院江苏南京211100

甲醛是一种比较常见的室内污染物,长期接触甲醛会危害人体健康.如何在低温条件下有效去除低浓度甲醛仍然是当前具有挑战性的研究课题.本文采用第一性原理计算方法研究了甲醛分子在单原子催化剂(Ti原子修饰的单层MXene-Ti3C2O2)表面上的... 详细信息

甲醛是一种比较常见的室内污染物,长期接触甲醛会危害人体健康.如何在低温条件下有效去除低浓度甲醛仍然是当前具有挑战性的研究课题.本文采用第一性原理计算方法研究了甲醛分子在单原子催化剂(Ti原子修饰的单层MXene-Ti3C2O2)表面上的吸附和催化氧化性能.结果表明, Ti原子在Ti3C2O2表面的结合能和扩散能分别为-8.36和1.66 eV,说明Ti能够以单原子形式稳定分散在Ti3C2O2表面,而不会产生团簇现象.为了研究甲醛和氧气分子在Ti/Ti3C2O2上的吸附机理,我们计算了分波态密度(PDOS), Mulliken电荷分析以及分子轨道.结果表明, Ti原子修饰改变了Ti3C2O2表面上的电荷分布,甲醛分子和氧气分子都能接受自Ti原子处转移而来的电子成为电子受体,增强了吸附质和Ti/Ti3C2O2之间的相互作用,从而加强了吸附能力.此外,为了研究甲醛分子在Ti/Ti3C2O2上的催化氧化机理,我们考虑了Langmuir-Hinshelwood (LH)和Eley-Rideal (ER)两种机理.结果表明,无论是从动力学还是热力学角度, ER机理是一种更为理想的催化氧化甲醛的方式,甲醛分子在已经被氧气活化的Ti/Ti3C2O2上能够自动解离成CO分子,而两个H原子则和活化的O原子形成两个*OH基团,并且释放4.05 eV的热量,从而有助于克服后续反应所要跨越的能垒(1.04 eV).而从*OH基团到CO分子的电荷转移不仅能够促进*OH基团的活化,而且也为下一步的水分子的形成也提供了重要作用.综上所述,甲醛可以很容易地在单原子催化剂Ti/Ti3C2O2上被氧化.综上,本文为开发高效去除甲醛的非贵金属催化剂以及扩大MXene材料应用范围提供重要指导.

关键词：甲醛氧化 MXene Ti/Ti3C2O2 单原子催化剂非贵金属催化剂

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莱州花岗岩应变岩爆实验声发射频谱特征分析

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地下空间与工程学报 2018年第1期14卷 51-57页

作者：贾雪娜姜全果何满潮任富强杜帅山东交通学院交通土建工程学院济南250357 山东省地质测绘院济南250002 深部岩土力学与地下工程国家重点实验室(北京) 北京100083 中国矿业大学(北京)力学与建筑工程学院北京100083 滨州学院山东滨州256600

深部岩爆的发生对应着岩石的猛烈破坏,同时产生弹性应力波,相应的就会有声发射现象发生。声发射频谱特征的变化能够反映岩爆发生的本质信息,因此开展此方面的研究有着重要的理论与应用价值。利用自主研发的深部岩爆过程模拟实验系统,进... 详细信息

深部岩爆的发生对应着岩石的猛烈破坏,同时产生弹性应力波,相应的就会有声发射现象发生。声发射频谱特征的变化能够反映岩爆发生的本质信息,因此开展此方面的研究有着重要的理论与应用价值。利用自主研发的深部岩爆过程模拟实验系统,进行了花岗岩循环加卸载条件下的岩爆声发射模拟实验。首先对花岗岩的应变岩爆实验过程进行划分,分析其声发射释能特征;其次,选取实验过程中的关键特征点声发射波形信息并对其进行傅里叶变换,观察各关键特征点的原始波形特征、二维频谱特征,寻求岩爆时刻的本征频谱;从其二维频谱功率谱图上,获取各个关键特征点的频谱响应特征和其对应的幅值特征,研究其频谱响应规律。研究结果表明:岩爆时刻区别于其他阶段最明显的特点就是声发射表现为连续型波形,低频高幅值特征。

关键词：花岗岩应变岩爆实验声发射傅里叶变换本征频谱

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Phase Behavior of Ionic Liquids-Cesium Carbonate-Water Aqueous Two-phase Systems and Their Extraction of L-Tryptophan

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Chemical Research in Chinese Universities 2018年第1期34卷 127-131页

作者： LI Shuang LI Shuni ZHAI quanguo jiang Yueheng HU Mancheng Key Laboratory of Macromolecular Science of Shaanxi Province School of Chemistry and Chemical Engineering Shaanxi Normal University Xi'an 710119 P. R. China

Phase behavior and extraction ability of aqueous two-phase systems（ATPs） consisting of ionic liquids（ILs）, Cs2CO3 and water were investigated in this paper. Four kinds of ionic liquids, namely, 1-amyl-3-methylimidazolium bromide（[Csmim]Br）, 1-hexyl-3-methylimidazolium bromide（[C6nim]Br）, 1-heptyl-3-methylimidazolium bromide （[C7mim]Br） and 1-octyl-3-methylimidazolium bromide（[C8mim]Br）, were examined to discuss the influence of alkyl groups. Binodal curves and tie-lines at 288.15, 298.15 and 308.15 K were obtained. The partitioning behavior for L-tryptophan in such ATPs was further investigated. The effect of temperature, pH, Cs2CO3 concentration and the structure of ionic liquids on the partitioning were discussed in detail.

关键词： Aqueous two-phase system Ionic liquid Cs2CO3 Partitioning behavior

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