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Tandem catalysis in electrocatalytic nitrate reduction:Unlocking efficiency and mechanism

Interdisciplinary Materials 2024年第2期3卷 245-269页

作者： Ziyang Wu Yanhui Song Haocheng Guo Fengting Xie Yuting Cong Min Kuang Jianping Yang State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghaiChina Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuanChina Helmholtz-Institute Ulm(HIU) UlmGermany

The electrochemical nitrate reduction reaction(NO_(3)RR)holds promise for ecofriendly nitrate ***,the challenge of achieving high selectivity and efficiency in electrocatalyst systems still significantly hampers the mechanism understanding and the large-scale *** catalysts,comprising multiple catalytic components working synergistically,offer promising potential for improving the efficiency and selectivity of the *** review highlights recent progress in designing tandem catalysts for electrochemical NO_(3)RR,including the noble metal-related system,transition metal electrocatalysts,and pulsed electrocatalysis ***,the optimization of active sites,interface engineering,synergistic effects between catalyst components,various in situ technologies,and theory simulations are discussed in *** and opportunities in the development of tandem catalysts for scaling up electrochemical NO_(3)RR are further discussed,such as stability,durability,and reaction *** outlining possible solutions for future tandem catalyst design,this review aims to open avenues for efficient nitrate reduction and comprehensive insights into the mechanisms for energy sustainability and environmental safety.

关键词： efficiency electrocatalytic nitrate reduction mechanism selectivity tandem catalysts

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Metal oxides heterojunction derived Bi-In hybrid electrocatalyst for robust electroreduction of CO_(2) to formate

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Journal of Energy Chemistry 2023年第8期83卷 180-188,I0007页

作者： Runze Ye Jiaye Zhu Yun Tong Dongmei Feng Pengzuo Chen School of Chemistry and Chemical Engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018ZhejiangChina

Electrochemical reduction of Bi-based metal oxides is regarded as an effective strategy to rationally design advanced electrocatalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR).Realizing high selectivity at high current density is important for formate production,but remains ***,the BiIn hybrid electrocatalyst,deriving from the Bi2O3/In2O3heterojunction(MOD-Biln),shows excellent catalytic performance for CO_(2)*** Faradaic efficiency of formate(FEHCOO-) can be realized over 90% at a wide potential window from-0.4 to-1.4 V ***,while the partial current density of formate(jHCOO-) reaches about 136.7 mA cm^(-2)at-1.4 V in flow cell without *** additio n,the MOD-Biln exhibits superior stability with high selectivity of formate at 100 mA cm^(-2).Systematic characterizations prove the optimized catalytic sites and interface charge transfer of MOD-Biln,while theoretical calculation confirms that the hybrid structure with dual Bi/In metal sites contribute to the optimal free energy of*H and*OCHO intermediates on MOD-Biln surface,thus accelerating the formation and desorption step of*HCOOH to final formate *** work provides a facile and useful strategy to develop highly-active and stable electrocatalysts for CO_(2)RR.

关键词： Metal oxide derivation Hybrid electrocatalyst Dual metal sites Electrocatalytic CO_(2)RR Formate product

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Layer-by-layer enriching active Ni-N_(3)C sites in nickel-nitrogen-carbon electrocatalysts for enhanced CO_(2)-to-CO reduction

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Chinese Chemical Letters 2023年第12期34卷 333-338页

作者： Yongqi Ren Ruopeng Chang Xu Hua Junjie Guo Guangping Hao Anhui Lu State Key Laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsLiaoning Key Laboratory for Catalytic Conversion of Carbon ResourcesSchool of Chemical EngineeringDalian Universityof TechnologyDalian 116024China Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuan 030024China

Transition metal and nitrogen co-doped carbons(M-N-C)have proven to be promising catalysts for CO_(2)electroreduction into co because of the high activity and *** enrichment of the active transition metal coordinated nitrogen sites is desirable but is challenging for a practical volumetric ***,we report four kinds of model electrocatalysts to unveil this issue,which include the NC structures with surface N-functionalities,Ni-N-CI with one layer of surface Ni-NsC sites,NC@Ni-N-CI with surface N-functionalities and underneath Ni-N3C sites as well as Ni-N-C_II with doubled surface Ni-NsC *** X-ray absorption spectroscopy indicates the coordination configuration of *** NC catalysts,when N-doping level increased from 3.5 at%to 8.4 at%,the CO partial current density increased from below 0.1 mA/cm^(2)to 3 mA/cm^(2).Introducing one layer of Ni-N_(3)C onto the NC structures leads to a 54 times higher CO partial current density than that of NC,in the meantime the FE_(CO) is 66 times ***,doubling the density of surface Ni-N_(3)C sites by a layer-by-layer method doubles the CO partial current density Gco,indicating its potential to achieve a high density of active coordinated sites and current densities.

关键词： Porous carbons Nanocarbons CO_(2)electroreduction M-N_(3)C structure Nonprecious electrocatalysts

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Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction

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Nano Research 2024年第6期17卷 4807-4814页

作者： Runze Chen Xiaoying Wang Jianfei Dang Songjie Yun Liqiang Wang Fangong Kong You-Nian Liu State Key Laboratory of Biobased Material and Green Papermaking Qilu University of TechnologyJinan 250353China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Hunan Provincial Key Laboratory of Micro&Nano Materials Interface Science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation,but the mechanism is still ***,nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom(Co1/NC)was taken as a model to uncover the mechanism of the reversible deactivation ***1/NC exhibited moderate adsorption towards the substrate molecules(i.e.,nitro compounds or related intermediates),which could be strengthened by the confinement effect from the porous ***,substrate molecules tend to accumulate within the pore channel,especially micropores that host Co1,making it difficult for the reactants to access the active sites and finally leading to their *** situation could be even worse when the substrate molecules possess a large ***,the catalytic activity of Co1/NC could be restored via a simple thermal treatment,which could remove the adsorbates within the pore channel,hence releasing active sites that were originally inaccessible to reactants.

关键词： single-atom catalysts porous carbon support reversible deactivation mechanistic study hydrogenation reaction

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Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

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Nano Research 2024年第3期17卷 1056-1065页

作者： Ke Yan Liang Chen Yangguang Hu Ting Wang Cong Chen Chao Gao Youju Huang Benxia Li School of Chemistry and Chemical Engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(H_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,H_(2)O dissociation and proton transfer is hardly achieved on a ***,the sluggish H_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer ***,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to *** photocatalytic CO_(2) reduction with H_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated *** H_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction *** kinetic isotope experiments indicate that the sluggish H_(2)O dissociation affects the whole photocatalytic CO_(2) reduction *** presence of oxygen vacancies promotes the adsorption and activation of H_(2)O and CO_(2),and the doped S sites play a crucial role in boosting H_(2)O dissociation and accelerating the dynamic migration of hydrogen *** a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance.

关键词： BiOCl sulfur doping photocatalytic CO_(2)reduction H_(2)O activation proton feeding

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Microstructure Evolution and Nanomechanical Behavior of Micro-Area in Molten Pool of Selective Laser Melting(CoCrNi)_(82)Al_(9)Ti_(9)High-Entropy Alloy

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Acta Metallurgica Sinica(English Letters) 2024年第6期37卷 1019-1033页

作者： Hong-Wei Zhang Li-Wei Lan Zhe-Yu Yang Chang-Chun Li Wen-Xian Wang College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan030024China Ministry of Education Key Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of TechnologyTaiyuan030024China Shanxi-Zhejiang University New Materials and Chemical Research Institute Taiyuan030032China

In this work,the phase evolution mechanism and nanomechanical properties of(CoCrNi))(82)Al_(9)Ti_(9)high-entropy alloy(HEA)prepared by selective laser melting(SLM)in the molten pool were *** HEA contains multiple primary elements and undergoes high-temperature gradient and rapid cooling during *** leads to significant inhomogeneity of nano-scale microstructure characteristics and instability of *** optimizing process parameters,the microstructure evolution at the optimal parameter volume energy density of 440 J/mm^(3)was studied.A phase transition from BCC to FCC occurred in the melt *** the micro-area of the melt pool results in a temperature rise and the combustion-induced loss of Al ***,the Ni element content increases significantly outside the melt *** process enhances the phase stability of FCC and facilitates phase ***,rapid cooling leads to the formation of distinctive ultrafine equiaxial crystals inside the melt pool,accompanied by the generation of intracrystalline needle-like nano-scale *** the melt pool,the accumulation of energy results in the formation of coarse ***,the nano-hardness inside the molten pool is remarkably high at 11.79 GPa,while the outside the molten pool is reduced to 9.58 *** the fracture toughness outside the melt pool also *** with inside the melt pool,the residual stress outside the melt pool changed from compressive to tensile stress and decreased from 603.28 to 322.84 MPa.

关键词： High-entropy alloys Selective laser melting Microstructure evolution Nanoindentation

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Identifying the origin of porous evolution of microsized bismuth in potassium-ion batteries

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science China Chemistry 2024年第7期67卷 2234-2239页

作者： Shenxu Chu Kaixiang Lei Qian Yang Jiaxin Li Yuqing Zhao Mengjia Gu Lin Li Xing Hu Yu Zhang Zhuo Chen Shuo Shi Shulei Chou Shijian Zheng Tianjin Key Laboratory of Materials Laminating Fabrication and Interface Control Technology School of Materials Science and EngineeringHebei University of TechnologyTianjin 300401China Institute for Carbon Neutralization Technology College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Microsized bismuth(Bi)with in-situ constructed three-dimensional(3D)porous network has been considered as a promising anode for high-performance potassium-ion batteries(PIBs).However,the mechanism of the in-situ porous evolution of microsized Bi during the charge/discharge process is still ***,various electrolytes are employed to disclose the origin of porous evolution of microsized Bi in *** and theoretically,the 3D porous network originates from the uniform interfacial charge distribution on the Bi surface in the linear ether-based *** addition,the universality of the interfacial charge distribution mechanism was verified by microsized Sn and *** in-situ constructed 3D porous network of Bi enables a superior potassium storage performance in a wide temperature range from-40 to 40℃.More importantly,the K_(0.9)Mn_(0.7)Ni_(0.3)O_(2)||Bi full cell delivers excellent cycling stability(a high capacity retention of 88.44%even after 2,000 cycles)and good temperature *** work gives a distinct clarification of the origin of the porous evolution of microsized Bi during cycling,which is critical for developing high-performance PIBs.

关键词： potassium-ion batteries microsized Bi porous evolution linear ether-based electrolyte interfacial charge distribution

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Immobilizing Triphenylamine with Photoredox Inert Sr^(2+)Forming Sr-MOF with Controlled Electron Migration for Photocatalytic Oxidation of Thiols to Disulfides

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Chinese Journal of Chemistry 2024年第10期42卷 1093-1099页

作者： Ying-Xia Wang Fang Zheng Dong-Xia Song Bao-Yue Niu Lu-Qian Deng Xian-Ming Zhang Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education) Schoolof Chemistry and Materials ScienceShanxi Normal UniversityTaiyuanShanxi 030006China Key Laboratory of Interface Science and Engineering in Advanced Material(Ministry of Education) College of ChemistryTaiyuan University of TechnologyTaiyuanShanxi 030024China

The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the *** and its derivatives(TPAs)are promising for the above reaction,but suffer from the easy polymerization and difficult *** overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates,herein,we constructed one TPA-based metal-organic framework(MOF),(Me_(2)NH_(2))[Sr(TCBPA)]·DMA·3H_(2)O(1),by direct self-assembly of tris(4′-carboxybiphenyl)amine(H_(3)TCBPA)and photoredox inert strontium ion(Sr^(2+)).DFT calculations revealed that the valence band maximum(VBM)and the conduction band minimum(CBM)are mainly located on TCBPA^(3-),successfully inhibiting the undesirable electron migration to metal *** results indicated that 1 displays superior performance than homogeneous H_(3)TCBPA,which may result from the abundant π…π and C—H…π interactions between the well-arranged TCBPA^(3-)and the build-in electric field between the anionic framework and the Me_(2)NH^(2+).This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

关键词： Triphenylamine Metal-organic frameworks Strontium Photooxidation Thiols Disulfides

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Influence of pH value on corrosion behavior of non-equiatomic Fe_(40)Mn_(20)Cr_(20)Ni_(20) high-entropy alloy

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Journal of Iron and Steel Research International 2025年第4期32卷 1114-1124页

作者： Zhen Wang Jun-feng Duan Jun-wei Qiao Hong-yan Che Xi-kou He Central Iron and Steel Research Institute Co. Ltd.Beijing100083China College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan030024ShanxiChina Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuan030024ShanxiChina

The electrochemical performance and corrosion properties of Fe_(40)Mn_(20)Cr_(20)Ni_(20) high-entropy alloys(HEAs)in a 3.5%NaCl solution with various pH values were thoroughly *** results revealed a close correlation between the corrosion properties of HEAs and the pH *** the one hand,the pH value can affect the semiconducting properties of the passive film on the alloy surfaces,thereby further influencing the protective capacity of the passive *** the other hand,an excess of H+or OH−promotes the growth of localized corrosion,facilitating the formation of a larger number of larger-sized localized corrosion ***,the corrosion of HEAs is most severe in acidic solutions.

关键词： Fe_(40)Mn_(20)Cr_(20)Ni_(20)alloy Corrosion mechanism High-entropy alloy pH value Passive film

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Recent advances in switchable surfactants for heavy oil production:A review

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Energy Geoscience 2024年第4期5卷 75-88页

作者： Qi Li Lingfei Liu Dejun Sun Zhenghe Xu Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinanShandong250100PR China Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials Department of Materials Science and EngineeringSouthern University of Science and TechnologyShenzhenGuangdong518055PR China Key Laboratory of Tertiary Oil Recovery and Oilfield Chemistry PetroChina Dagang Oilfield CompanyTianjin300280PR China

Surfactants are extensively employed in the cold production of heavy ***,producing heavy oil emulsions using conventional surfactants poses a challenge to spontaneous demulsification,necessitating the addition of demulsifiers for oil-water *** inevitably increases the exploitation cost and environmental pollution *** surfactants have garnered much attention due to their dual capabilities of underground heavy oil emulsification and surface *** study focuses on the fundamental working principles and classification of novel switchable surfactants for oil displacement developed in recent *** offers a comprehensive overview of the latest advances in the applications of switchable surfactants in the fields of enhanced oil recovery(EOR),oil sand washing,and oil-water ***,it highlights the existing challenges and future development directions of switchable surfactants for heavy oil recovery.

关键词： Heavy oil Switchable surfactant Cold production Emulsification Demulsification

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