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Tandem catalysis of Cu/Ni multi-sites promotes oxygen reduction reaction

Science China Materials 2024年第9期67卷 2934-2940页

作者： Bin-Bin Feng Ke-Ke Chang Wan-Feng Xiong duan-hui si Shui-Ying Gao Hong-Fang Li Rong Cao College of Chemistry and Materials Science Fujian Normal UniversityFuzhou350007China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China University of Chinese Academy of Sciences Beijing100049China

The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon(M-N-C)materials have made them extremely attractive for oxygen reduction reactions(ORRs).However,it is inevitable that hydrogen peroxide(H_(2)O_(2))will be formed via the two-electron pathway in ***,the Cu nanoparticles(NPs)have been encapsulated into Ni doped hollow mesoporous carbon spheres(Ni-HMCS)to reduce the generation of H_(2)O_(2)in *** tests confirm that the introduction of Cu NPs improves the ORR performance *** obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V *** hydrogen electrode and a limited current density of 5.5 mA cm^(-2),which is comparable with the commercial Pt/***,Cu/Ni-HMCS has been used in Zn-air battery,demonstrating a high power density of 161 mW cm^(-2)and a long-term recharge capability(50 h at 5 mA cm^(-2)).The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis,that is,H_(2)O_(2)released from the Ni-N_(4)and Cu-N_(4)sites migrates to the Cu(111)face,on which the captive H_(2)O_(2)is further reduced to H_(2)*** work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR,which provides an insight into the development of effective fuel cell electrocatalysts.

关键词： oxygen reduction reaction tandem catalysis pathway dual-metal multi-sites Cu nanoparticles

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Conductive phthalocyanine-based metal-organic framework as a highly efficient electrocatalyst for carbon dioxide reduction reaction

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Science China Chemistry 2021年第8期64卷 1332-1339页

作者： Meng-Di Zhang duan-hui si Jun-Dong Yi Qi Yin Yuan-Biao Huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Sciences Beijing100049China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou350007China Fujian College University of Chinese Academy of SciencesFuzhou350002China

Porous crystalline metal-organic frameworks(MOFs)are one class of promising electrode materials for CO_(2)electroreduction reaction(CO_(2)RR)by virtue of their large CO_(2)adsorption capacities and abundant tunable active sites,but their insulating nature usually leads to low current ***,a two-dimensional(2D)Ni-phthalocyanine-based MOF(NiPc-Ni(NH)4)constructed by 2,3,9,10,16,17,23,24-octaaminophthalocyaninato nickel(II)(NiPc-(NH_(2))_(8))and nickel(II)ions attained high electrical conductivity due to the high overlap of d-πconjugation orbitals between the nickel node and the Ni-phthalocyanine-substituted *** CO_(2)RR,the NiPc-Ni(NH)4 nanosheets achieved a high CO Faradaic efficiency of 96.4%at−0.7 V and a large CO partial current density of 24.8 mA cm^(−2)at−1.1 V,which surpassed all the reported two-dimensional MOF electrocatalysts evaluated in an *** control experiments and density functional theory(DFT)calculations suggested that the Ni-N_(4)units of the phthalocyanine ring are the catalytic active *** work provides a new route to the design of highly efficient porous framework materials for the enhanced electrocatalysis via improving electrical conductivity.

关键词： metal-organic frameworks electroreduction conductive CO_(2) CO

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Highly efficient electroreduction of CO_(2) by defect single-atomic Ni-N_(3) sites anchored on ordered micro-macroporous carbons

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Science China Chemistry 2022年第8期65卷 1584-1593页

作者： Qiu-Xia Li duan-hui si Wan Lin Yao-Bing Wang Hong-Jing Zhu Yuan-Biao Huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry Fuzhou UniversityFuzhou 350108China University of the Chinese Academy of Sciences Beijing 100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Microporous supports typically fail to fully expose active sites for electrolytes and CO_(2) molecules,and this usually results in low current density for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).To overcome the biggest obstacle and facilitate commercial applications,defective single-atomic Ni-N_(3) sites anchored to ordered micro-macroporous N-doped carbon(Ni-N/OMC)have been prepared by the pyrolysis of the Ni-ZIF-8@PS(ZIF=zeolitic imidazolate framework)and are intended to provide enhanced CO_(2)RR with a current density at an industrial *** Ni-ZIF-8@PS is constructed of nickel-based ZIF-8 embedded in the three-dimensional(3D)highly ordered polystyrene spheres(PS).The 3D ordered micro-macroporous architecture of Ni-N/OMC could facilitate the mass transfer of substrates to the accessible defective single-atomic Ni-N_(3) sites through micropores(0.6 nm)and macropores(~200 nm)interconnected by 50 nm *** a flow cell,Ni-N/OMC exhibits almost 100.0%CO Faraday efficiency(FECO)between−0.2 and−1.1 V *** and an industrial level CO partial current density of 208 mA cm^(−2).It has a turnover frequency of 1.5×10^(5) h^(−1) at−1.1 V *** in 1 M KOH electrolyte,which exceeds that of most reported nickel-based *** excellent CO_(2)RR performance for Ni-N/OMC makes it a state-of-the-art electrocatalyst for CO_(2)*** calculations show that the defective Ni-N_(3) site can lower the energy of*COOH formation compared with that of the Ni-N4 site,thereby accelerating CO_(2)***-N/OMC can also be utilized as a cathodic catalyst in Zn-CO_(2) battery,exhibiting high CO selectivity in the discharge process and excellent *** work paves a pathway to rational design of highly efficient electrocatalysts with 3D hierarchically ordered micro-macroporous architecture for CO_(2)RR towards industrial production and commercial applications.

关键词： metal-organic framework hierarchically ordered porous carbon Ni single atom CO_(2)electrocatalysis CO

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Boosting Electrocatalytic CO_(2)Reduction with Conjugated Bimetallic Co/Zn Polyphthalocyanine Frameworks

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CCS Chemistry 2023年第5期5卷 1130-1143页

作者： Nan Li duan-hui si Qiu-jin Wu Qiao Wu Yuan-Biao Huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of Chinese Academy of Science Beijing 100049 Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108

Development of high-efficiency electrode materials for the electrochemical CO_(2)reduction reaction(CO_(2)RR)with high current density and selectivity compatible with industry is an important but significant ***,we describe a facile strategy to enhance the selectivity and current density by regulating the local electron density of the cobalt site in a series of stable,conjugated,bimetallic Co/Zn polyphthalocyanine frameworks Co_(x)Zn_(y)PPc with an AB stacking model under alkaline aqueous *** adjusting the ratio of Co and Zn to 3:1,the optimal Co3Zn1PPc exhibits an industry-compatible CO partial current density of 212 mA cm^(−2)at−0.9 V versus reversible hydrogen electrode in a flow cell,which is 1.7 and 9.1 times that of the single metal polyphthalocyanine CoPPc and ZnPPc,***_(3)Zn_(1)PPc shows a high CO Faraday efficiency of more than 90%in a wide operating potential window of−0.3 to−0.9 ***-depth experimental and theoretical analysis revealed that introduction of electron-rich Zn atoms modified the electron density of the active Co center,placing Co in the electronrich region and weakening the bonding strength with the reaction intermediate,thereby improving the CO_(2)RR *** results clarify the interaction mechanism of dual metal sites at the atomic level and provide a new avenue for the design of electrocatalysts with potential in industrial applications.

关键词： CO_(2)electrocatalysis flow cell cobalt polyphthalocyanine zinc polyphthalocyanine AB stacking

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Ni single-atom sites supported on carbon aerogel for highly efficient electroreduction of carbon dioxide with industrial current densities

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eScience 2022年第3期2卷 295-303页

作者： hui Guo duan-hui si Hong-Jing Zhu Qiu-Xia Li Yuan-Biao Huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Sciences Beijing100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian350108China

Finding highly efficient electrocatalysts for the CO_(2)electroreduction reactions(CO_(2)RR)that have high selectivity and appreciable current density to meet commercial application standards remains a *** their reduction potentials are similar to that of the associated competitive hydrogen evolution reaction and the CO_(2)activation kinetics are *** single-atom catalysts(SACs)with high atom efficiency are one class of promising candidates for the CO_(2)RR to produce CO,single-atom active sites supported on microporous carbons are not fully exposed to substrates and thus lead to low current *** aerogels with interconnected channels and macropores can facilitate mass *** few reports describe utilizing them as supports to anchor SACs for efficient ***,N-doped carbon aerogels supporting Ni single atomic catalyst sites(denoted as Ni-NCA-X,X¼10,20)were fabricated by pyrolyzing Ni/Zn bimetallic zeolitic imidazolate framework(Ni/Zn-ZIF-8)/carboxymethylcellulose composite *** to abundant hierarchical micro-,meso-,and macropores and high CO_(2)adsorption,the Ni single active sites in the optimal Ni-NCA-10 were readily accessible for the electrolyte and CO_(2)molecules and thus achieved an industrial-level CO partial current density of 226 mA cm?2,a high CO Faradaic efficiency of 95.6%at?1.0 V *** reversible hydrogen electrode,and a large turnover frequency of 271810 h?1 in a flow-cell reactor at?1.0 *** excellent CO_(2)RR performance makes Ni-NCA-10 a rare state-of-the-art electrocatalyst for CO_(2)-to-CO *** work provides an effective strategy for designing highly efficient electrocatalysts toward the CO_(2)RR to achieve industrial current density via anchoring single-atom sites on carbon aerogels.

关键词： Carbon aerogel ZIF-8 single-atom catalyst CO_(2)electrocatalysis CO

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Energy-efficient buffer and service rate allocation in manufacturing systems using hybrid machine learning and evolutionary algorithms

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Advances in Manufacturing 2024年第2期12卷 227-251页

作者： si-Xiao Gao hui Liu Jun Ota Key Laboratory of Traffic Safety on Track of Ministry of Education Institute of Artificial Intelligence and Robotics(IAIR)School of Traffic and Transportation EngineeringCentral South UniversityChangsha410075People’s Republic of China Research into Artifacts Center for Engineering School of EngineeringThe University of TokyoTokyoJapan

Currently,simultaneous buffer and service rate allocation is a topic of interest in the optimization of manufacturing *** allocation problems have been solved previously to satisfy economic requirements;however,owing to the progress of green manufacturing,energy conservation and environmental protection have become increasingly ***,an energy-efficient approach is developed to maximize the throughput and minimize the energy consumption of manufacturing systems,subject to the total buffer capacity,total service rate,and predefined energy *** energy-efficient approach integrates the simulated annealing-non-dominated sorting genetic algorithm-II with the honey badger algorithm-histogram-based gradient boosting regression *** former algorithm searches for Pareto-optimal solutions of sufficient *** latter algorithm builds prediction models to rapidly calculate the throughput,energy consumption,and energy *** examples show that the proposed hybrid approach can achieve a better solution quality compared with previously reported ***,the prediction models can rapidly evaluate manufacturing systems with sufficient *** study benefits the multi-objective optimization of green manufacturing systems.

关键词： Energy-efficient allocation Multi-objective optimization Energy efficiency Energy consumption Machine learning

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Enhancement of Ising superconductivity in monolayer NbSe_(2) via surface fluorination

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Science China(Technological Sciences) 2024年第7期67卷 2099-2106页

作者： WU JiZheng SHI WuJun WANG Chong duan Wenhui XU Yong si Chen School of Materials Science and Engineering Beihang UniversityBeijing 100191China Center for Transformative Science ShanghaiTech UniversityShanghai 201210China Shanghai High Repetition Rate XFEL and Extreme Light Facility(SHINE) ShanghaiTech UniversityShanghai 201210China State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics Tsinghua UniversityBeijing 100084China Frontier Science Center for Quantum Information Beijing 100084China

Recently discovered Ising superconductors have garnered considerable interest due to their anomalously large in-plane upper critical fields(B_(c2)). However, the requisite strong spin-orbital coupling in the Ising pairing mechanism generally renders these superconductors heavy-element dominant with notably low superconducting transition temperatures(Tc). Here, based on the Migdal-Eliashberg theory and the mean-field Bogoliubov-de Gennes Hamiltonian, we demonstrate a significant enhancement of Ising superconductivity in monolayer NbSe_(2) through surface fluorination, as evidenced by concomitant improvements in Tcand Bc_(2). This enhancement arises from three predominant factors. Firstly, fluorine atoms symmetrically and stably adhere to both sides of the monolayer NbSe_(2), thereby maintaining the out-of-plane mirror symmetry and locking carrier spins ***, fluorination suppresses the charge density wave in monolayer NbSe_(2) and induces a van Hove singularity in the vicinity of the Fermi level, leading to a marked increase in the number of carriers and, consequently, strengthening the electron-phonon coupling(EPC). Lastly, the appearance of fluorine-related, low-frequency phonon modes further augments the EPC. Our findings suggest a promising avenue to elevate Tcin two-dimensional Ising superconductors without compromising their Ising pairing.

关键词： Ising superconductivity surface functionalization upper critical field NbSe_(2) first-principles calculations

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Structure and 2p decay mechanism of^(18)Mg

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Nuclear Science and Techniques 2024年第6期35卷 145-154页

作者： Long Zhou De-Qing Fang si-Min Wang hui Hua Key Laboratory of Nuclear Physics and Ion-beam Application(MOE) Institute of Modern PhysicsFudan UniversityShanghai 200433China Shanghai Research Center for Theoretical Nuclear Physics NSFC and Fudan UniversityShanghai 200438China School of Physics and State Key Laboratory of Nuclear Physics and Technology Peking UniversityBeijing 100871China

The recently discovered,extremely proton-rich nuclide 18 Mg exhibits ground-state decay via two sequential two-proton(2p)emissions through the intermediate nucleus,*** study investigates the structure and the initial 2p decay mechanism of^(18)Mgby examining the density and correlations of the valence protons using a three-body Gamow coupled-channel *** results show that the ground state of^(18)Mgis significantly influenced by the continuum,resulting in a significant s-wave ***,based on the current framework,this does not lead to a significant deviation in mirror symmetry in either the structure or spectroscopy of the 18Mg-18C ***,the time evolution analysis of the^(18)Mgground state suggests a simultaneous 2p emission during the first step of *** observed nucleon-nucleon correlations align with those of the light-mass 2p emitters,indicating a consistent decay behavior within this nuclear region.

关键词： Structure of^(18)Mg Two-proton decay Proton-proton correlation

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Crystalline-amorphous M@MN_x(M=Co,Fe,Ni)encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： Yang Yang Xiao-Chuan duan Shao-hui Guo Xian-Ming Zhang College of Materials Science and Engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of TechnologyYuci030600China

Developing earth-abundant electrocatalysts for hydrogen evolution reaction(HER)is important for the sustainable energy ***,efficient and stable heterocatalysts consisting of crystalline-amorphous M@MN_(x)(M=Co,Fe,Ni)encapsulated in N-doped carbon layers supported with N-doped graphene sheets(denoted as M@MN_(x)@NC-NG)are synthesized by facile hydrothermal reaction and nitridation *** the nitriding process,metal ions in M(tzbc)_2(H_(2)O)_4(tzbc=4-(1H-1,2,4-triazol-1-yl)benzoic acid)complexes are reduced to crystalline M cores,accompanied by the formation of amorphous MN_(x)shells;the tzbc ligands are insitu carbonized to form outermost N-doped carbon(NC)layers that connect with inner MN_(x)via M-N-C motifs inherited from the complex precursors and inhibit the transition of MN_(x)from amorphous to crystalline *** Co@CoN_(x)@NC-NG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm^(-2)and low Tafel slopes of 40 and 85 mV·dec^(-1)in 0.5 mol·L^(-1)H_(2)SO_4 and1.0 mol·L^(-1)KOH electrolytes,*** Co@CoN_(x)@NC-NG retains 97%of the initial overpotential after 100,000 s in both acidic and alkaline *** outstanding HER performance originates from the crystalline-amorphous Co@CoN_(x)that redistributes electrons around the heterointerfaces,facilitating the conversion process of H^(+)/H_(2)O to hydrogen and thereby promoting HER *** outermost NC layers serve as the armor of Co@CoN_(x),and graphene nanosheets act as carriers of egg-like Co@CoN_(x)@NC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

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Super-high bed sintering for iron ores: inhomogeneous phenomena and its mechanism during mineralizing

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Journal of Iron and Steel Research International 2024年第8期31卷 1850-1860页

作者： hui-bo Liu Liang-ping Xu Xi-duan Yang Zhong-lin Dong Qiang Zhong Guang-hui Li School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083HunanChina

The inhomogeneous sinter properties in super-high bed sintering have been reported in our previous *** inves-tigate the reasons for the inhomogeneous phenomena,detailed sampling and analysis of mixed material bed and sintered bed in super-high bed sintering plant were *** results indicated that the higher porosity and thinner dendrite of silico-ferrite of calcium and aluminum in the upper layer as well as dense structure and higher secondary hematite content in the lower layer led to the heterogeneities of mechanical strength and reduction properties exceeding 20%and 10%,*** the bed top downward,the basicity of mixed material decreased from 2.13 to 1.68 because the average particle size increased from 2.65 to 4.56 *** and fuels gathered in finer particles(-3 mm)of mixed material,and the-3 mm particles of mixed material generated more liquid phase than+3 mm *** heat input of super-high sintering bed was inhomogeneous due to the heat accumulation effect and unreasonable fuel *** inhomo-geneous sintering heat condition in sintering bed resulted in the different quantities and properties of liquid *** inhomogeneous quantities and properties of liquid phase that were influenced by inhomogeneous distribution of chemical composition,particle size,and heat input led to inhomogeneous mineralizing *** mineralizing condition is the key for homogeneous super-high bed sintering.

关键词： Iron ore Super-high bed sintering Mineralization Material segregation Heat accumulation

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