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In-situ reconstruction of catalysts in cathodic electrocatalysis: New insights into active-site structures and working mechanisms

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Journal of Energy Chemistry 2022年第7期31卷 414-436,I0011页

作者： Wenbiao Zhang Yang Yang Yi Tang qingsheng gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632GuangdongChina Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsLaboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials(iCHEM)Fudan UniversityShanghai 200433China

Cathodic electrocatalytic reactions, such as hydrogen evolution and CO_(2)/N_(2) reduction, are the key processes that store intermittent electricity into stable chemical energy. Although a great progress has been made to boost activity and selectivity via elaborative catalyst design, the structure–property relationships have not been sufficiently understood in the context of surface reconfiguration under working conditions. Recent efforts devoted to tracking dynamic evolution of electrocatalysts using in-situ and/or operando techniques gave new insights into the real structure and working mechanism of active sites,and provided principles to design better catalysts. The achievement of cathodic electrocatalysts in this subject is herein summarized, focusing on the correlations between reconstructed surface and electrocatalytic performance. Briefly, the thermodynamics of reconstruction at cathodes is discussed at first, and then the representative progresses in H_(2) evolution and CO_(2)/N_(2) reduction are introduced in sequence to acquire insights into electrochemical processes on in-situ reconfigured surfaces or interfaces. Finally, a perspective is offered to guide future investigations. This review is anticipated to shed some new light on in-depth understanding cathodic electrocatalysis and exploiting prominent electrocatalysts.

关键词： Hydrogen evolution reaction CO_(2)reduction reaction Nitrogen reduction reaction In-situ reconstruction Electronic configurations Valence states Topological changes

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Recent advances of two-dimensional CoFe layered-double-hydroxides for electrocatalytic water oxidation

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Chinese Chemical Letters 2022年第6期33卷 2845-2855页

作者： Yi Zhou Jialai Hu Lichun Yang qingsheng gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China School of Materials Science and Engineering and Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640China Ningbo Fengcheng Advanced Energy Materials Research Institute Co. Ltd.Ningbo 315000China

Oxygen evolution reaction(OER)is pivotal to drive green hydrogen generation from water electrolysis,but yet is strictly overshadowed by the sluggish reaction ***-abundant and cut-price transitionmetal compounds,particularly Co Fe layered-double-hydroxides(LDHs),show the distinct superiorities in contrast to noble metals and their *** this review,we firstly underline their fundamental issues in electrocatalytic water oxidation,including Co Fe LDHs crystal structure,the surface of(hydr)oxides confined to OER and the controversial roles of Fe species,aiming at understanding the structure-related activity and catalytic *** approaches for optimizing OER activity of Co Fe LDHs are then comprehensively overviewed,which will shed light on the different working mechanisms and provide a concise analysis of their unique ***,a perspective on the future development of Co Fe LDHs electrocatalysts is *** hope this review can give a concise and explicit guidance for the development of transition-metal-based electrocatalysts in the energy field.

关键词： CoFe layered-double-hydroxides Electrocatalytic water oxidation Two-dimensional nanostructures Surface reconstruction d-band

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Phase Engineering of CoMo0_(4)Anode Materials toward Improved Cycle Life for Li^(+)Storage

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Chinese Journal of Chemistry 2021年第5期39卷 1121-1128页

作者： Xiaoqing Huang Junhao Li Wenbiao Zhang Wenjie Huang Lichun Yang qingsheng gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhouGuangdong 510632China School of Materials Science and Engineering and Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhouGuangdong 510641China

Anode materials based on conversion reactions usually possess high energy densities for lithium-ion batteries(LIBs).However,they suffer from poor rate performance and cycle life due to serious volume ***,α/β-CoMo04 heterogeneous nanorods are synthesized via a facile co-precipitation method,and further are phase-engineered through varying calcination temperature,accomplishing the obviously improved cycle life and rate performance as anodes for *** evaluated at a current density of 1.0 A·g^(-1)the optimal nanorods with anα/βphase ratio of 6.0 afford the reversible capacity of 1143.6 mAh·g^(-1)after 200 cycles,outperforming most of recently reported bimetal ***^(+)storage mechanism is further analyzed by using in-situ X-ray diffraction and ex-situ transition electronic ***'s revealed thatβ-CoMoO_(4)follows a one-step conversion reaction;whileα-CoMo0_(4)proceeds an intercalation pathway before the conversion *** storage of Li^(+)would alleviate the volume effect of heterostructuredα/β-CoMo0_(4),forming electronically conductive network evenly composed of Co and Mo nanograins to enable the reversible electrochemical *** work is anticipated to give some hints for the rational design of high-performance energy materials.

关键词： Electrochemistry Anode materials Bimetal oxides Crystal engineering Reaction mechanisms

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Binding SnO_(2)Nanoparticles with MoS_(2)Nanosheets Toward Highly Reversible and Cycle-Stable Lithium/Sodium Storage

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Energy & Environmental Materials 2024年第4期7卷 135-142页

作者： Deliang Cheng Wenbiao Zhang Yi Tang qingsheng gao Renzong Hu Lichun Yang Min Zhu Institute of Advanced Materials Jiangxi Normal UniversityNanchang 330022China School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510641China College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsLaboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200433China

SnO_(2),with its high theoretical capacity,abundant resources,and environmental friendliness,is widely regarded as a potential anode material for lithium-ion batteries(LIBs).Nevertheless,the coarsening of the Sn nanoparticles impedes the reconversion back to SnO_(2),resulting in low coulombic efficiency and rapid capacity *** this study,we fabricated a heterostructure by combining SnO_(2)nanoparticles with MoS_(2)nanosheets via plasma-assisted *** heterostructure consists of in-situ exfoliated MoS_(2)nanosheets predominantly in 1 T phase,which tightly encase the SnO_(2)nanoparticles through strong *** configuration effectively mitigates the volume change and particle aggregation upon ***,the strong affinity of Mo,which is the lithiation product of MoS_(2),toward Sn plays a pivotal role in inhibiting the coarsening of Sn nanograins,thus enhancing the reversibility of Sn to SnO_(2)upon ***,the SnO_(2)/MoS_(2)heterostructure exhibits superb performance as an anode material for LIBs,demonstrating high capacity,rapid rate capability,and extended ***,discharged/charged at a rate of 0.2 A g^(-1)for 300 cycles,it achieves a remarkable reversible capacity of 1173.4 mAh g^(-1).Even cycled at high rates of 1.0 and 5.0 A g^(-1)for 800 cycles,it still retains high reversible capacities of 1005.3 and 768.8 mAh g^(-1),***,the heterostructure exhibits outstanding electrochemical performance in both full LIBs and sodium-ion batteries.

关键词： 1 T-MoS_(2) heterostructure lithium-ion batteries Sn coarsening SnO_(2)

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Metal-encapsulated nitrogen-doped carbon nanotube arrays electrode for enhancing sulfion oxidation reaction and hydrogen evolution reaction by regulating of intermediate adsorption

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Chinese Chemical Letters 2024年第8期35卷 533-538页

作者： Xiao Li Wanqiang Yu Yujie Wang Ruiying Liu Qingquan Yu Riming Hu Xuchuan Jiang qingsheng gao Hong Liu Jiayuan Yu Weijia Zhou Institute for Advanced Interdisciplinary Research(iAIR) School of Chemistry and Chemical EngineeringUniversity of JinanJi’nan 250022China Institute for Smart Materials&Engineering School of Materials Science and EngineeringUniversity of JinanJi’nan 250022China College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China State Key Laboratory of Crystal Materials Shandong UniversityJi’nan 250100China

For treatment of sulfion-containing wastewater,coupling the electrochemical sulfion oxidation reaction(SOR)with hydrogen evolution reaction(HER)can be an ideal way for sulfur and H_(2)resources ***,we synthesize a metal-modified carbon nanotube arrays electrode(Co@N-CNTs/CC)for SOR and *** electrode has excellent performance for SOR and HER attributed to the unique array *** can achieve 99.36 mA/cm^(2)at 0.6 V for SOR,and 10 mA/cm^(2)at 0.067 V for *** functional theory calculations verify that metal modification is able to regulate the electronic structure of carbon nanotube,which is able to optimize the adsorption of *** Co@N-CNTs/CC as bifunctional elec-trodes to establish a hybrid electrolytic cell can reduce about 67%of energy consumption compared with the traditional water splitting electrolytic ***,the hybrid electrolytic cell is used to treat actual sulfion-containing wastewater,achieving the sulfur yield of 30 mg h^(−1)cm^(−2)and the hydrogen production of 0.64 mL/min.

关键词： Sulfion oxidation reaction Hydrogen evolution reaction Nitrogen-doping carbon nanotube Core-shell structure Resource upgrade

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Revealing Real Facet Effect（{100}, {110} and {111}） of Palladium Nanocrystals for Biosensing

Revealing Real Facet Effect（{100}, {110} and {111}） of Pal...

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中国化学会第二十次全国电化学大会

作者： Yang Yang qingsheng gao College of Chemistry and Materials Science Jinan University

Pd nanomaterials are widely used as a type of highly sensitive non-enzyme electrochemical biosensors. And its synthesis is usually assisted by various types of surfactants. Unfortunately, the residual surfactants is inevitably changing activity of electrochemical sensing because active sites are occupied by ligands such as halide ion and/or long-chain alkyl. Hence, removing these ligands is significant for realizing their intrinsic functions.

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Nickel-doped CoN nanowire bundles as efficient electrocatalysts for oxygen evolution reaction

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Science China Materials 2021年第8期64卷 1889-1899页

作者： Dan Li Wenbiao Zhang Jiachang Zeng Boxu gao Yi Tang qingsheng gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsLaboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200433China

Cost-efficient electrocatalysts composed of earth-abundant elements are highly desired for enhanced oxygen evolution reaction (OER).As a promising candidate,metallic Co4N already demonstrated electrocatalytic performance relying on specific nanostructures and electronic ***,nickel was introduced as the dopant into one-dimensional (1D) hierarchical Co4N structures,achieving effective electronic regulation of Co4N toward high OER *** amount of Co3+increased after Ni-doping,and the in-situ formed surface oxyhydroxide during OER enhanced the electrocatalytic ***,the 1D hierarchical structure further promoted the performances of Co4N owing to the high electrical conductivity and abundant activesites on the rough *** expected,the optimal Ni-doped Co4N with a Ni/Co molar ratio of 0.25 provides a small overpotential of 233 mV at a current density of 10 mA cm^(-2),with a low Tafel slope of 61 mV dec^(-1),and high long-term stability in 1.0 mol L^(-1)*** these results,the enhancement by doping the Co4N nanowire bundles with Fe and Cu was further evidenced for the OER.

关键词： oxygen evolution reaction cobalt nitrides heteroatom doping electronic state nanowire bundles

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Facet dependence of electrocatalytic furfural hydrogenation on palladium nanocrystals

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Chinese Journal of Catalysis 2022年第12期43卷 3116-3125页

作者： Wenbiao Zhang Yanghao Shi Yang Yang Jingwen Tan qingsheng gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632GuangdongChina State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510640GuangdongChina

Electrocatalytic hydrogenation(ECH)offers a sustainable route for the conversion of biomass-derived feedstocks under ambient conditions;however,an atomic-level understanding of the catalytic mechanism based on heterogeneous electrodes is *** gain insights into the relation between electrocatalysis and the catalyst surface configuration,herein,the facet dependence of the ECH of furfural(FAL)is investigated on models of nanostructured Pd cubes,rhombic dodecahedrons,and octahedrons,which are predominantly enclosed by{100},{110},and{111}facets,*** facet-dependent specific activity to afford furfuryl alcohol(FOL)follows the order of{111}>{100}>{110}.Experimental and theoretical kinetic analyses confirmed the occurrence of a competitive adsorption Langmuir-Hinshelwood mechanism on Pd,in which the ECH activity can be correlated with the difference between the binding energies of chemisorbed H(^(*)H)and FAL(^(*)FAL)based on density functional theoretical(DFT)*** the three facets,Pd{111}exhibiting the strongest^(*)H but the weakest^(*)FAL showed the copresence of the^(*)H and^(*)FAL intermediates on the Pd surface for subsequent hydrogenation,experimentally confirming its high ECH activity and Faradaic *** free energies determined using DFT calculations indicated that^(*)H addition to the carbonyl of FAL on Pd{111}was thermodynamically preferred over desorption to gaseous H2,contributing to efficient ECH to afford FOL at the expense of H2 *** obtained insights into the facet-dependent ECH underline that surface bindings assist ECH or H2 evolution considering their *** findings are expected to deepen the fundamental understanding of electrochemical refinery and broaden the scope of electrocatalyst exploration.

关键词： Electrocatalytic hydrogenation Furfural Pd nanocrystal Facet dependence Binding energy

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撤案权与监督撤案权的行使边界

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人民检察 2010年第4期 14-18页

作者：高庆盛浙江省人民检察院

撤案权的行使主体为侦查机关,行使条件为"发现不应对犯罪嫌疑人追究行使责任";行使阶段为侦查过程中;行使对象为不符合立案条件而立案侦查的案件和符合立案条件但经侦查终结应当撤销的案件。监督撤案权的主体为检察机关,具体为侦查监督... 详细信息

撤案权的行使主体为侦查机关,行使条件为"发现不应对犯罪嫌疑人追究行使责任";行使阶段为侦查过程中;行使对象为不符合立案条件而立案侦查的案件和符合立案条件但经侦查终结应当撤销的案件。监督撤案权的主体为检察机关,具体为侦查监督部门;监督撤案权的行使阶段为侦查阶段;对侦查机关应当撤案而不撤案的案件监督其撤案,必须符合两个条件:一是案件在撤案权的行使边界内;二是监督撤案权的行使须具有监督必要性。不得行使监督撤案权的情形包括:刑事和解案件,具有从轻、减轻或免除处罚情节但已构成犯罪的案件;审查起诉环节发现不应当追究刑事责任的案件;符合公安机关立案标准,尚在侦查中的案件;同一犯罪嫌疑人实施多起犯罪行为,需要并案侦查的案件;对同一犯罪嫌疑人以多个罪名立案侦查,其中部分罪名不构罪的;以事立案尚未确定犯罪嫌疑人的;不构成犯罪不捕后七日内的案件。

关键词：撤案权监督撤案权行使主体行使情形

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Interlayer engineering of molybdenum disulfide toward efficient electrocatalytic hydrogenation

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Science Bulletin 2021年第10期66卷 1003-1012,M0004页

作者： Jingwen Tan Wenbiao Zhang Yijin Shu Haiyang Lu Yi Tang qingsheng gao College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsLaboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials(iCHEM)Fudan UniversityShanghai 200433China

Electrocatalytic hydrogenation(ECH)enables the sustainable production of chemicals under ambient condition;however,suffers from serious competition with hydrogen(H2)evolution and the use of precious metals as ***,molybdenum disulfide is for the first time developed as an efficient and noble-metal-free catalyst for ECH via in situ intercalation of ammonia or alkyl-amine *** interlayer engineering regulates phase transition(2H→1 T),and effectively ameliorates electronic configurations and surface hydrophobicity to promote the ECH of biomass-derived oxygenates,while prohibiting H2 *** optimal one intercalated by dimethylamine(MoS_(2)-DMA)is capable of hydrogenating furfural(FAL)to furfuryl alcohol with high Faradaic efficiency of 86.3%–73.3%and outstanding selectivity of>95.0%at−0.25 to−0.65 V(***),outperforming MoS_(2) and other conventional *** prominent performance stems from the enhanced chemisorption and surface *** chemisorption of H intermediate and FAL,synchronously strengthened on the edge-sites of MoS_(2)-DMA,accelerates the surface elementary step following Langmuir-Hinshelwood ***,the improved hydrophobicity benefits FAL affinity to overcome diffusion *** the effective modulation of MoS_(2) from a typical H2 evolution electrocatalyst to a promising candidate for ECH,this study broadens the scope to exploit catalysts used for electrochemical synthesis.

关键词： Electrocatalytic hydrogenation Molybdenum disulfide Interlayer engineering Binding energy Surface hydrophobicity

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