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hydrogen spillover bridged dual nano-islands triggered by built-in electric field for efficient and robust alkaline hydrogen evolution at ampere-level current density

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Nano Research 2024年第6期17卷 5050-5060页

作者： Kecheng Tong Liangliang Xu Hanxu Yao Xingkun Wang Canhui Zhang Fan Yang Lei Chu Jinwoo Lee Heqing Jiang Minghua Huang School of Materials Science and Engineering Ocean University of ChinaQingdao 266100China Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology(KAIST)291Daejeon 34141Republic of Korea Qingdao New Energy Shandong Laboratory Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China University of Chinese Academy of Sciences Beijing 100049China

Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operating at ampere-level current density.Herein,the unique Ru and RuP_(2)dual nano-islands are deliberately implanted on N-doped carbon substrate(denoted as Ru-RuP_(2)/NC),in which a built-in electric field(BEF)is spontaneously generated between Ru-RuP_(2)dual nano-islands driven by their work function difference.Experimental and theoretical results unveil that such constructed BEF could serve as the driving force for triggering fast hydrogen spillover process on bridged Ru-RuP_(2)dual nano-islands,which could invalidate the inhibitory effect of high hydrogen coverage at ampere-level current density,and synchronously speed up the water dissociation on Ru nano-islands and hydrogen adsorption/desorption on RuP_(2)nano-islands through hydrogen spillover process.As a result,the Ru-RuP_(2)/NC affords an ultra-low overpotential of 218 mV to achieve 1.0 A·cm^(−2)along with the superior stability over 1000 h,holding the great promising prospect in practical applications at ampere-level current density.More importantly,this work is the first to advance the scientific understanding of the relationship between the constructed BEF and hydrogen spillover process,which could be enlightening for the rational design of the cost-effective alkaline HER catalysts at ampere-level current density.

关键词： built-in electric field hydrogen spillover dual nano-islands ampere-level current density alkaline hydrogen evolution

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hydrogen spillover in nonreducible oxides:Mechanism and catalytic utilization

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Nano Research 2022年第12期15卷 10357-10365页

作者： Songhyun Lee Hyungjun Kim Ryong Ryoo Jeong Young Park Minkee Choi Charles D.Davidson School of Chemical Engineering Purdue UniversityWest LafayetteIndiana47907USA Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and TechnologyDaejeon34141Republic of Korea Department of Chemistry Korea Advanced Institute of Science and TechnologyDaejeon34141Republic of Korea KENTECH Laboratory for Chemical Environmental and Climate TechnologyKorea Institute of Energy Technology(KENTECH)200 Hyeoksin-roNaju58330Republic of Korea Center for Nanomaterials and Chemical Reactions Institute for Basic Science(IBS)Daejeon34141Republic of Korea

hydrogen(H)spillover in nonreducible oxides such as zeolites and Al2O3 has been a highly controversial phenomenon in heterogeneous catalysis.Since industrial catalysts are predominantly prepared using these materials as supports,it is important to understand the mechanism and catalytic functions of H spillover on their surfaces.In the past decade,fundamental studies on zeolite-encapsulated metal catalysts have revealed that H spillover and reverse spillover can be utilized in the design of hydrogenation and dehydrogenation catalysts with improved properties.Both experimental and theoretical studies have indicated that H spillover can occur in nonreducible oxides when they possess substantial acid sites that aid the surface migration of active H.In the present review,we will discuss the possible mechanisms of H spillover in nonreducible oxides and the unique opportunities of using this phenomenon for the design of advanced hydroprocessing catalysts.

关键词： hydrogen spillover nonreducible oxides zeolites hydroprocessing catalysts

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Magic of hydrogen spillover: Understanding and application

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Green Energy & Environment 2022年第6期7卷 1161-1198页

作者： Haifang Shen Hao Li Zhensheng Yang Chunli Li National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of Technology8 Guangrong RoadTianjin300130China

The hydrogen spillover effect(HSPE)plays an important role in heterogeneous catalysis and hydrogen storage as an interfacial phenomenon,which facilitates the improvement of hydrogen storage properties of porous nanomaterials and indirectly or directly affects the reaction performance of multiphase catalytic reactions.The setting-up of the word“hydrogen spillover”opened up a new area to gain insight into the dynamic behavior of migrating hydrogen atoms on a catalyst surface.However,a comprehensive understanding of the HSPE is still lacking.Today,the development of advanced characterization techniques provides increasingly valuable information to further our understanding of the HSPE.Based on these considerations,in this review,we hope to provide some answers to the question“What is hydrogen spillover and how do we recognize it?”.To do this,we will rely on advanced characterization techniques as well as experimental and theoretical studies.Then,we discuss in detail the influences of the HSPE on hydrogen storage performance and the important catalytic effects of the HSPE in catalysis.These effects will be reviewed by looking through the catalytic results obtained in many reactions in thermal catalysis,electrocatalysis,and photocatalysis.Furthermore,based on the application potential of hydrogen spillover,we present some preliminary research proposals and discuss the opportunities and challenges that remain to be faced in this research area.

关键词： hydrogen spillover Characterization hydrogen storage Catalysis spillover mechanism

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Atomically Dispersed Pt and NiO Clusters Synergistically Enhanced C–O Bond hydrogenolysis

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CCS Chemistry 2024年第3期6卷 709-718页

作者： Junjuan Yang Sen Luan Minghua Dong Yuxuan Wu Xueqing Xing Xingwu Liu Junfeng Xiang Zhijuan Zhao Shaopeng Li Bin Zhang Huizhen Liu Buxing Han Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsBeijing 100049 National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Huairou DistrictBeijing 101400 Center for Physicochemical Analysis and Measurement Institute of ChemistryChinese Academy of SciencesBeijing 100190 Physical Science Laboratory Huairou National Comprehensive Science CenterUniversity of Chinese Academy of SciencesBeijing 100049

C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and biomass.Developing efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic utilization.Herein,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO clusters.The synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly clarified.These findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.

关键词： bimetallic catalysis synergistic effect C-O bond activation hydrogenolysis hydrogen spillover

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Construction of pH-universal hydrogen evolution freeway in MoO_(3)-MoNi_(4)@Cu core-shell nanowires via synergetic electronic and geometric effect

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Nano Research 2023年第10期16卷 12253-12262页

作者： Xiaodong Chen Shoufu Cao Xiaojing Lin Xiaofei Wei Zhaojie Wang Hongyu Chen Chengcheng Hao Siyuan Liu Shuxian Wei Daofeng Sun Xiaoqing Lu School of Materials Science and Engineering China University of Petroleum(East China)Qingdao 266580China College of Science China University of Petroleum(East China)Qingdao 266580China

Both the adsorption/dissociation of water molecules and hydrogen intermediate(H*)are the major limitations to hydrogen evolution reaction(HER).Herein,the modulation of electronic structure and geometric configuration are combined to design onedimensional electrocatalyst with outstanding HER activity in a wide pH range.The catalyst was composed of molybdenum trioxide doped molybdenum nickel alloy supported by copper nanowires(MoO_(3)-MoNi_(4)@Cu NWs).As revealed by the experimental characterizations and theoretical calculations,Cu NWs act as the electron donator to MoNi4,resulting in up shift of the d-band center in MoNi4,thus expediting H_(2)O adsorption and dissociation.Moreover,the introduction of amorphous MoO_(3) sets up a unique geometric configuration on MoNi4 for the accelerated H*transfer via hydrogen-bond and hydrogen spillover.This work provides a synergetic route for constructing HER freeway and promotes further investigations on more versatile electrocatalysis involving H_(2)O or H*.

关键词： pH-universal hydrogen evolution reaction(HER) electronic structure geometric configuration hydrogen-bond hydrogen spillover

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Light doping of tungsten into copper-platinum nanoalloys for boosting their electrocatalytic performance in methanol oxidation

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Nano Research Energy 2022年第2期1卷 194-200页

作者： Danye Liu Qing Zeng Chaoquan Hu Dong Chen Hui Liu Yongsheng Han Lin Xu Qingbo Zhang Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100China School of Chemistry and Materials Science Jiangsu Key Laboratory of New Power BatteriesJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjing 210023China Department of Bioengineering Rice UniversityHoustonTexas 77005USA

Coupling the bi-functional mechanism with compressive lattice strain might be an effective way to boost the electrocatalysis of platinum(Pt)-based nanoparticles for methanol oxidation reaction(MOR).This strategy weakens the chemisorption of poisoning CO-like intermediates generated during MOR on the active Pt sites by lowering their d-band center.In this context,we herein report the synthesis of ternary copper-tungsten-platinum(CuWPt)nanoalloys with light doping of W element by simply co-reducing their precursors at elevated temperature.In this ternary alloy system,the presence of only small amount of W element not only weakens the chemisorption of CO-like intermediates by lowering the Pt d-band center through compressive lattice strain,but also cleans the active Pt sites by“hydrogen spillover effect”,endowing the as-prepared CuWPt nanoalloys at an appropriate Cu/W/Pt ratio with good activity for MOR.In specific,the ternary CuWPt alloy nanoparticles at a Cu/W/Pt molar ratio of 21/4/75 show a specific activity of 2.5 mA·cm^(−2)and a mass activity of 2.11 A·mg^(−1)with a better durability,outperforming those ternary CuWPt alloy nanoparticles at other Cu/W/Pt ratios,binary CuPt alloys and commercial Pt/C catalyst as well as a large number of reported Pt-based electrocatalysts.In addition,a single direct methanol fuel cell(DMFC)assembled using ternary CuWPt nanoalloys as anodic catalysts shows a power density of 24.3 mW·cm^(−2)and an open-circle voltage of 0.6 V,also much higher than those of the single DMFC assembled from commercial Pt/C catalysts.

关键词： lattice strain d-band center electrocatalysis hydrogen spillover methanol oxidation reaction

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Theoretical study of molecular hydrogen and spiltover hydrogen storage on two-dimensional covalent-organic frameworks

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Chinese Physics B 2014年第6期23卷 493-500页

作者：刘秀英何杰于景新栗正新樊志琴 College of Science Henan University of Technology School of Material Science and Engineering Henan University of Technology

Molecular hydrogen and spiltover hydrogen storages on five two-dimensional （2D） covalent-organic frameworks （COFs）（PPy-COF, TP-COF, BTP-COF, COF-18 A, and HHTP-DPB COF） are investigated using the grand canonical Monte Carlo （GCMC） simulations and the density functional theory （DFT）, respectively. The GCMC simulated results show that HHTP-DPB COF has the best performance for hydrogen storage, followed by BTP-COF, TP-COF, COF-18 A, and PPy-COE However, their adsorption amounts at room temperature are all too low to meet the uptake target set by US Department of Energy （US-DOE） and enable practical applications. The effects of pore size, surface area, and isosteric heat of hydrogen on adsorption amount are considered, which indicate that these three factors are all the important factors for determining the H2 adsorption amount. The chemisorptions of spiltover hydrogen atoms on these five COFs represented by the cluster models are investigated using the DFT method. The saturation cluster models are constructed by considering all possible adsorption sites for these cluster models. The average binding energy of a hydrogen atom and the saturation hydrogen storage density are calculated. The large average binding energy indicates that the spillover process may pro- ceed smoothly and reversibly. The saturation hydrogen storage density is much larger than the physisorption uptake of H2 molecules at 298 K and 100 bar （1 bar = 105 Pa）, and is close to or exceeds the 2010 US-DOE target of 6 wt% for hydrogen storage. This suggests that the hydrogen storage capacities of these COFs by spillover may be significantly enhanced. Thus 2D COFs studied in this paper are suitable hydrogen storage media by spillover.

关键词： hydrogen spillover covalent-organic frameworks hydrogen storage grand canonical Monte Carlo simulation

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TiO_(2) nanorods based self-supported electrode of 1T/2H MoS_(2) nanosheets decorated by Ag nano-particles for efficient hydrogen evolution reaction

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Chinese Chemical Letters 2023年第11期34卷 355-359页

作者： Changzheng Lin Yunpeng Liu Yaxing Sun Zhenyu Wang Hao Xu Mingtao Li Jiangtao Feng Bo Hou Wei Yan Department of Environmental Science&Engineering Xi’an Jiaotong UniversityXi’an 710049China School of Physics and Astronomy Cardiff UniversityThe ParadeCardiffCF243AAWalesUnited Kingdom State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049China International Research Center for Renewable Energy(IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering(MFPE)Xi’an Jiaotong UniversityXi’an 710049China

Molybdenum disulfide(MoS_(2))has shown significant promise as an economic hydrogen evolution reaction(HER)catalyst for hydrogen generation,but its catalytic performance is still lower than noble metalbased catalysists.Herein,a silver nanoparticles(Ag NPs)-decorated 1T/2H phase layered MoS_(2) electrocatalyst grown on titanium dioxide nanorod arrays(Ag NPs/1T(2H)MoS_(2)/TNRs)was prepared through acid-tunable ammonium ion intercalation.Taking advantage of MoS_(2) layered structure and crystal phase controllability,as-prepared Ag NPs/1T(2H)MoS_(2)/TNRs exhibited ultrahigh HER activity.As-proposed strategy combines facile hydrogen desorption(Ag NPs)with efficient hydrogen adsorption(1T/2H MoS_(2))effectively circumventes the kinetic limitation of hydrogen desorption by 1T/2H MoS_(2).The as-prepared Ag NPs/1T(2H)MoS_(2)/TNRs electrocatalyst exhibited excellent HER activity in 0.5 mol/L H2SO4 with low overpotential(118 mV vs.reversible hydrogen electrode(RHE))and small Tafel slope(38.61 mV/dec).The overpotential exhibts no obvious attenuation after 10 h of constant current flow.First-principles calculation demonstrates that as-prepared 1T/2H MoS_(2) exhibit a large capacity to store protons.These protons can be subsequently transferred to Ag NPs,which significantly increases the hydrogen coverage on the surface of Ag NPs in HER process and thus change the rate-determining step of HER on Ag NPs from water dissociation to hydrogen recombination.This study provides a unique strategy to improve the catalytic activity and stability for MoS_(2)-based electrocatalyst.

关键词： Molybdenum disulfide Silver nanoparticles hydrogen evolution reaction Density functional theory hydrogen spillover

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Synergetic effect between sulfurized Mo/γ-Al_2O_3 and Ni/γ-Al_2O_3 catalysts in hydrodenitrogenation of quinoline

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Journal of Natural Gas Chemistry 2011年第2期20卷 214-217页

作者： Lihua Liu Bin Liu Yongming Chai Yunqi Liu Chenguang Liu State Key Laboratory of Heavy Oil Processing Key Laboratory of Catalysis CNPC China University of Petroleum （East China） Qingdao 266555 Shandong China

An evidence for the synergetic effect between the stacked bed of Mo/γ-Al2O3 and Ni/γ-Al2O3 in the hydrodenitrogenation （HDN） reaction of quinoline has been provided in this paper. The synergism factor decreases when the reaction temperature increases （280？340 ？C）. The synergetic effect leads to improve the hydrogenation activity for the stacked bed compared with the single Mo/γ-Al2O3 bed, which may be attributed to the generation of hydrogen spillover on the Ni/γ-Al2O3 catalyst.

关键词： hydrogen spillover synergetic effect hydrodenitrogenation NiMo catalyst

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