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Journal of Energy Chemistry 2024年第4期91卷 27-35页

作者： Yonghai Feng Min Yu Minjia Meng Lei Liu dewei rao Institute for Advanced Materials School of Materials Science and EngineeringJiangsu UniversityZhenjiang 212013JiangsuChina School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina

In the selective oxidation of biomass-based 1,2-propanediol(PDO)with oxygen as the terminal oxidant,it is challenging to improve the lactic acid(LA)selectivity for nonnoble metal nanoparticles(NPs)due to their limited oxygen reduction rate and easy C-C *** the high economic feasibility of nonnoble metals,i.e.,Cu,in this work,copper and nitrogen codoped porous carbon nanosheets encapsulating ultrafine Cu nanoparticles(Cu@Cu-N-C)were developed to realize highly selective of PDO oxidation to *** carbon-encapsulated ultrasmall Cu^(0)NPs in Cu@Cu-N-C have high PDO dehydrogenation activity while N-coordinated Cu(Cu-N)sites are responsible for the high oxygen reduction ***,the performance of catalytic PDO conversion to LA is optimized by a proposed pathway of PDO→hydroxylacetone→lactaldehyde→***,the enhanced LA selectivity is 88.5%,and the PDO conversion is up to 75.1%in an O_(2)-pressurized reaction system(1.0 MPa O_(2)),superior to other Cu-based catalysts,while in a milder nonpressurized system(O_(2)flow rate of 100 mL min-1),a remarkable LA selectivity(94.2%)is obtained with 39.8%PDO conversion,2.2 times higher than that of supported Au nanoparticles(1%Au/C).Moreover,carbon encapsulation offers Cu@Cu-N-C with strong leaching resistance for better recycling.

关键词： Selective oxidation Copper and nitrogen doped carbon 1,2-Propanediol Ultrasmall Cu nanoparticles Lactic acid

Strong coupled spinel oxide with N-rGO for high-efficiency ORR/OER bifunctional electrocatalyst of Zn-air batteries

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Journal of Energy Chemistry 2021年第6期30卷 428-435,I0011页

作者： Wenjun Liu dewei rao Jian Bao Li Xu Yucheng Lei Huaming Li School of Material Science&Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina Institute for Energy Research Jiangsu UniversityZhenjiang 212013JiangsuChina

The high cost,scarcity,and poor stability of precious-metal-based catalysts have hindered their extensive application in energy conversion and *** stimulates the search for earth-abundant alternatives to replace noble metal ***,in this study,we investigate a novel and low-cost bifunctional electrocatalyst consisting of ZnCoMnO_(4) anchored on nitrogen-doped graphene oxide(ZnCoMnO_(4)/N-rGO).Benefiting from the strong Co-N interaction in ZnCoMnO_(4) and the coupled conductive N-rGO,the catalysts exhibit high electrocatalytic ***,density functional theory calculations support the dominant role of the strong Co-N electronic interaction,which leads to ZnCoMnO_(4)/N-rGO having more favorable binding energies with O2 and H_(2) O,resulting in fast reaction *** obtained ZnCoMnO_(4)/N-rGO electrocatalyst exhibits superb bifunctional activity,with a half-wave potential of 0.83 V for the oxygen reduction reaction and a low onset potential of 1.57 V for the oxygen evolution reaction in 0.1 M KOH ***,a Zn-air battery driven by the ZnCoMnO_(4)/N-rGO catalyst shows remarkable discharge/charge performance,with a power density of 138.52 mW cm^(-2) and longterm cycling stability for 48 *** work provides a promising multifunctional electrocatalyst based on non-noble metals for the storage and conversion of renewable energy.

关键词： Bifunctional catalyst Zn-air battery Spinel structure Synergistic effect Strong Co-N interaction

Selective and effective oxidation of 5-hydroxymethylfurfural by tuning the intermediates adsorption on Co-Cu-CN_(x)

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Nano Research 2023年第5期16卷 6670-6678页

作者： Tianyun Jing Shaokang Yang Yonghai Feng Tingting Li Yunpeng Zuo dewei rao School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China Institute of Surface Micro and Nano Materials Xuchang UniversityXuchang 461002China Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research InstitutePalackýUniversity77900 OlomoucCzech Republic Pharmaceutical Sciences Laboratory and Turku Bioscience Center Åbo Akademi UniversityTurku 20520Finland

Co-based catalysts are promising alternatives to precious metals for the selective and effective oxidation of 5-hydroxymethylfurfural(HMF)to the higher value-added 2,5-furandicarboxylic acid(FDCA).However,these catalysts still suffer from unsatisfactory activity and poor selectivity.A series of N-doped carbon-supported Co-based dual-metal nanoparticles(NPs)have been designed,among which the Co-Cu_(1.4)-CN_(x) exhibits enhanced HMF oxidative activity,achieving FDCA formation rates 4 times higher than that of pristine Co-CN_(x),with 100%FDCA *** functional theory(DFT)calculations evidenced that the increased electron density on Co sites induced by Cu can mediate the positive electronegativity offset to downshift the dband center of Co-Cu_(1.4)-CN_(x),thus reducing the energy barriers for the conversion of HMF to *** findings will support the development of superior non-precious metal catalysts for HMF oxidation.

关键词： Co-based materials 5-hydroxymethylfurfural(HMF)oxidative activity 2,5-furandicarboxylic acid(FDCA)selectivity electronegativity offset d-band center

Non-metallic electronic regulation in CuCo oxy-/thio-spinel as advanced oxygen evolution electrocatalysts

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Science China Chemistry 2021年第1期64卷 101-108页

作者： Huan Yang Shuai Gao dewei rao Chaonan Zhang Xuecheng Zhou Shaokang Yang Jingjing Ye Shasha Yang Feili Lai Xiaohong Yan School of Materials Science and Engineering Jiangsu UniversityZhenjicmg 212013China Department of Chemistry KU LeuvenCelestijnenlaan 200FLeuven 3001Belgium

Developing cost-effective and high-performance oxygen evolution reaction(OER)electrocatalysts has become the intense research on pursuing emerging renewable energy conversion,in which exploring and investigating the intrinsic nature of efficient and stable Cu Co spinel catalysts toward OER in alkaline media is highly ***,Cu1–xCo2+xO4oxy-spinel nanoflakes are fabricated by a facile hydrothermal method with the oxidation of ammonia *** the same condition,Cu1–xCo2+xS4thio-spinel nanospheres are formed without *** OER process,the as-obtained Cu1–xCo2+xO4nanoflakes and Cu1–xCo2+xS4nanospheres possess the anodic overpotential of 267 and 297 m V in alkaline media to drive the current density of 10 m A/cm^2,respectively,outperforming the state-of-the-art noble metal catalyst of RuO2.X-ray photoelectron spectroscopy analysis exhibits the higher ratio value of Co(Ⅲ)/Co(Ⅱ)in Cu1–xCo2+xO4than that in Cu1–xCo2+xS4,suggesting that the stronglyelectronegative oxygen efficiently predominates in regulating valence states of Co active sites in spinel ***,density functional theory simulation further reveals that the increased valence state of Co could accelerate the electron exchange between catalysts and oxygen adsorbates during electrocatalysis,thus contributing to the higher OER activity of Cu1–xCo2+*** work provides deep insight regarding the significance of non-metal element(O and S)in Cu Co spinel structure catalysts,as well as presents a promising approach to exploit higher performance and grasp the mechanism of various non-noblemetal spinel catalysts for water oxidation.

关键词： copper-cobalt oxy-spinel thio-spinel oxygen evolution reaction density functional theory

Cu_(2+1)O/CuO_(x)heterostructures promote the electrosynthesis of C^(2+)products from CO_(2)

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Nano Research 2023年第4期16卷 4698-4705页

作者： Rongbo Sun Cong Wei Zixiang Huang Shuwen Niu Xiao Han Cai Chen Haoran Wang Jia Song Jun-Dong Yi Geng Wu dewei rao Xusheng Zheng Yuen Wu Gongming Wang Xun Hong Center of Advanced Nanocatalysis(CAN) Department of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China National Synchrotron Radiation Laboratory(NSRL) University of Science and Technology of ChinaHefei 230026China

Manipulating the oxidation state of Cu catalysts can significantly affect the selectivity and activity of electrocatalytic carbon dioxide reduction(CO_(2)RR).However,the thermodynamically favorable cathodic reduction to metallic states typically leads to catalytic ***,a defect construction strategy is employed to prepare crystalline/amorphous Cu_(2+1)O/CuO_(x)heterostructures(c/a-CuO_(x))with abundant Cu0 and Cuδ+(0<δ<1)sites for CO_(2)*** C^(2+)Faradaic efficiency of the heterostructured Cu catalyst is up to 81.3%,with partial current densities of 406.7 mA·cm−***,real-time monitoring of the Cu oxidation state evolution by in-situ Raman spectroscopy confirms the stability of Cuδ+species under long-term high current density *** functional theory(DFT)calculations further reveal that the adjacent Cu0 and Cuδ+sites in heterostructured c/a-CuO_(x)can efficiently reduce the energy barrier of CO coupling for C^(2+)products.

关键词： CO_(2)electroreduction C-C coupling heterostructures in-situ Raman manipulation of oxidation states

Synergistic interaction of Nb atoms anchored on g‐C_(3)N_(4) and H^(+) promoting high‐efficiency nitrogen reduction reaction

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Chinese Journal of Catalysis 2022年第4期43卷 1139-1147页

作者： Shaokang Yang Chaonan Zhang dewei rao Xiaohong Yan School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina

Nowadays catalytic nitrogen reduction reaction(NRR)by electrochemistry has attracted much attention because of its key role in producing the basic chemical product ammonia with low energy consumption.A stable and environmentally‐friendly single‐or multi‐atom catalyst with good performance in activity and selectivity is highly desired for *** density functional theory calculations,the NRR mechanisms catalyzed by Nb monomer,dimer,trimer and tetramer anchored on graphitic carbon nitride(Nb_(x)@g‐C_(3)N_(4),x=1,2,3,4)have been deeply *** has been found that Nb_(3)@g‐C_(3)N_(4) exhibits the best catalytic ability among the four catalysts with the introduction of H+.A more stable intermediate(*NH_(2)+*H)can be found to reduce the huge free energy barrier of forming*NH_(3) from*NH_(2) directly in a multi‐atom *** analyzing the density of states and projected crystal orbital Hamilton population,a synergistic effect among Nb atoms and the adsorbed H^(+)is responsible for reducing the overpotential of ***,the competitive hydrogen evolution reaction is suppressed *** work introduces a new insight in the reaction pathway in multi‐atoms for developing high‐efficiency NRR catalysts.

关键词： Catalysis N_(2)fixation Nitrogen reaction H^(+)absorption Selectivity

Accelerating water dissociation kinetics of Ni3N by tuning interfacial orbital coupling

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Nano Research 2021年第10期14卷 3458-3465页

作者： Yishang Wu Yufang Xie Shuwen Niu Yipeng Zang Jinyan Cai Zenan Bian Xuanwei Yin Yanyan Fang Da Sun Di Niu Zheng Lu Amirabbas Mosallanezhad Huijuan Wang dewei rao Hongge Pan Gongming Wang Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei 230026China Experimental Center of Engineering and Material Science University of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China Institute of Science and Technology for New Energy Xi’an Technological UniversityXi’an 710021China School of Materials Science and Engineering State Key Laboratory of Silicon MaterialsZhejiang UniversityHangzhou 310027China

The high unoccupied d band energy of Ni_(3)N basically results in weak orbital coupling with water molecule,consequently leading to slow water dissociation ***,we demonstrate Cr doping can downshift the unoccupied d orbitals and strengthen the interfacial orbital coupling to boost the water dissociation *** prepared Cr-Ni_(3)N/Ni displays an impressive overpotential of 37 mV at 10 mA·cmgeo-2,close to the benchmark Pt/C in 1.0 M KOH *** structural analysis reveals the Cr dopant exists as the Cr-N_(6)states and the average d band energy of Ni_(3)N is also *** functional theory calculation further confirms the downshifted d band energy can strengthen the orbital coupling between the unpaired electrons in O 2p and the unoccupied state of Ni 3d,which thus facilitates the water adsorption and *** work provides a new concept to achieve on-demand functions for hydrogen evolution catalysis and beyond,by regulating the interfacial orbital coupling.

关键词： unoccupied d orbitals Ni_(3)N Cr-N_(6)doping interfacial orbital coupling hydrogen evolution reaction

Orbital-regulated interfacial electronic coupling endows Ni3N with superior catalytic surface for hydrogen evolution reaction

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Science China Chemistry 2020年第11期63卷 1563-1569页

作者： Yanyan Fang Da Sun Shuwen Niu Jinyan Cai Yipeng Zang Yishang Wu Linqin Zhu Yufang Xie Yun Liu Zixuan Zhu Amirabbas Mosallanezhad Di Niu Zheng Lu Junjie Shi Xiaojing Liu dewei rao Gongming Wang Yitai Qian Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science&Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China

The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation,which consequently results in weak orbital coupling with H2O and slow water dissociation kinetics for alkaline hydrogen evolution ***,we successfully lower the unoccupied d orbital energy of Ni3N to strengthen the interfacial electronic coupling by employing the strong electron pulling capability of oxygen *** prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm−2,very close to the commercial Pt/*** structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni ***,density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and *** concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.

关键词： hydrogen evolution reaction orbital regulation interfacial electronic coupling Ni3N electrocatalysts

Behavior of gold-enhanced electrocatalytic performance of NiPtAu hollow nanocrystals for alkaline methanol oxidation

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Science China Materials 2021年第3期64卷 611-620页

作者： Chang Liu Zelin Chen dewei rao Jinfeng Zhang Yunwei Liu Yanan Chen Yida Deng Wenbin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin300372China School of Materials Science and Engineering Jiangsu UniversityZhenjiang212013China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou350207China

The Pt-based catalyst tends to be poisoned by carbon monoxide(CO)-like intermediates produced in fuel cell reactions,which seriously deteriorates its catalytic ***,noble metal Au with the capacity of resistance to CO-like intermediates poisoning was employed to construct multi-element Pt-based *** trimetallic NiPtAu hollow nanocrystals(HNCs)with different surface Au contents were synthesized to explore the role of Au in electrocatalysis for alkaline methanol oxidation reaction(MOR).The trimetallic NiPtAu-SRAu HNCs catalyst with the relative rich Au content(15.17 at%)on surface exhibits a much lower CO oxidation peak potential than the other HNCs counterpart and 20 wt%Pt/C,which indicates the more exceptional CO-resisting ***,the MOR specific activity of NiPtAu-SRAu HNCs(31.52 mA cm^−2)is 7 times higher than that of 20wt%Pt/C(4.50 mA cm^−2).This enhancement in catalytic activity as well as anti-CO poisoning capability for NiPtAu-SRAu HNCs can be mainly ascribed to the weakened CO adsorption due to the exposure of Au atoms on NiPt surface evidenced by the experimental data and density functional theory *** study not only investigates the role of Au in MOR catalysis but also could be helpful for designing and optimizing the electrocatalysts for high-active and robust fuel cell applications.

关键词： trimetallic NiPtAu hollow nanocrystals methanol oxidation carbon monoxide poisoning

Hierarchical iridium-based multimetallic alloy with double-core-shell architecture for efficient overall water splitting

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Science China Materials 2020年第2期63卷 249-257页

作者： Jie Zhang Zelin Chen Chang Liu Jun Zhao Siliang Liu dewei rao Anmin Nie Yanan Chen Yida Deng Wenbin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin 300072China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China State Key Lab of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004China Joint School of National University of Singapore and Tianjin University Internatioal Campus of Tianjin UniversityFuzhou 350207China

The overall water splitting for hydrogen production is an effective strategy to resolve the environmental and energy crisis. Here, we report a facile approach to synthesize the Ir-based multimetallic, hierarchical, double-coreshelled architecture(HCSA) assisted by oil bath reaction for boosting overall water splitting in acidic environment. The Ir Ni Cu HCSA shows superior electrocatalytic activity for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER), which are comparable to commercial Pt/C and better than IrO2. The Ir Ni Cu HCSA exhibits remarkably catalytic efficiency as bifunctional catalyst for overall water splitting where a low cell voltage of 1.53 V is enough to drive a current density of 10 mA cm^-2 and maintains stable for at least 20 h. The presented work for the design and synthesis of novel Ir-based multimetallic architecture paves the way for highperformance overall water splitting catalysis.

关键词： IrNiCu nanoframe hierarchical structure core-shell oxygen evolution reaction hydrogen evolution reaction