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Journal of Energy Chemistry 2024年第3期90卷 388-411,I0010页

作者： Mostafa Tarek Janaina S.Santos Victor Márquez Mohammad Fereidooni Mohammad Yazdanpanah Supareak Praserthdam Piyasan Praserthdam center of Excellence on Catalysis and catalytic Reaction Engineering(CECC) Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailan High-Performance Computing Unit(CECC-HCU) Center of Excellence on Catalysis and Catalytic Reaction Engineering(CECC)Chulalongkorn UniversityBangkok 10330Thailand

Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low *** various technologies,the selective oxidation of hydrogen sulfide(SOH_(2)S) to elemental sulfur(S) has emerged as a sustainable and environmentally friendly *** to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH_(2)S;however,rapid deactivation has remained a significant *** causes of iron oxide-based catalysts deactivation mechanisms in SOH_(2)S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this *** focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH_(2)S.

关键词： Selective oxidation of H_(2)S Iron-based Catalysts Mechanism of deactivation Sulfur or sulfate deposition Transformation of iron species Sintering SDG 7

Combining anodic alcohol oxidative coupling for C-C bond formation with cathodic ammonia production

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National Science Review 2024年第5期11卷 217-226页

作者： Leitao Xu Wei Chen Cairong Wang Wenjie Wu Yelin Yao Zhifeng Huang Jingcheng Wu Ming Yang Yandong Wu Dianke Xie Yuqin Zou Shuangyin Wang State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of Education Hunan University

Electrocatalytic oxidation of alcohols using heterogeneous catalysts is a promising aqueous, energy-efficient and environmentally friendly approach, especially for coupling different alcohols to prolong the carbon chain via co-oxidation. Precisely regulating critical steps to tailor electrode materials and electrolyte composition is key to selectively coupling alcohols for targeted synthesis. However, selectively coupling different alcohols remains challenging due to the lack of effective catalyst and electrolyte design promoting specific pathways. Herein, we demonstrate a paired electrolysis strategy for combining anodic oxidative coupling of ethanol（EtOH） and benzyl alcohol（PhCH2OH） to synthesize cinnamaldehyde（CAL） and cathodic ammonia production. The strategies involve:（i） utilizing the salt-out effect to balance selective oxidation and coupling rates;（ii） developing platinum-loaded nickel hydroxide electrocatalysts to accelerate intermediate coupling kinetics;（iii） introducing thermodynamically favorable nitrate reduction at the cathode to improve coupling selectivity by avoiding hydrogenation of products while generating valuable ammonia instead of hydrogen. We achieved 85% coupling selectivity and 278 μmol/h NH3productive rate at 100 m A/cm2with a low energy input（～1.63 V）. The membrane-free, low energy, scalable approach with a wide substrate scope highlights promising applications of this methodology. This work advances heterogeneous electrocatalytic synthesis through rational design principles that integrate anodic oxidative coupling with cathodic nitrate reduction reactions, having synergistic effects on efficiency and selectivity.

关键词： anodic alcohol oxidative coupling C–C bond formation cinnamaldehyde cathodic ammonia production

Weak interaction-steered evolution of polyoxovanadate-based metal-organic polyhedra from transformation via interlock to packing

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Chinese Chemical Letters 2024年第2期35卷 527-533页

作者： Yan-Hu Wang Ke-Wei Tong Chao-Qin Chen Jing Du Peng Yang College of Chemistry and Chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China College of Chemistry and Materials Science Testing and Analysis CenterHebei Normal UniversityShijiazhuang 050024China

A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak *** contrast with covalent bonds bearing definite orientation and high stability,weak intermolecular forces within a continuous dynamic equilibrium can be hardly tamed for molecular *** this endeavor,a ligand-dominated strategy that embodies tunable electrostatic repulsion andπ···πstacking was first employed to shape polyoxovanadate-based metal-organic polyhedra(VMOPs).Structural evolution involving transformation,interlock,and discovery of an unprecedented prototype of the Star of David was hence *** only as a handy tool for the primary structural control over VMOPs,these weak forces allow for an advanced management on the spatial distribution of such manmade macromolecules as well as the associated physicochemical behaviors,representing an ideal model for simulating and interpreting the conformation-function relationship of proteins.

关键词： Polyoxometalates Polyoxovanadates Metal-organic polyhedron Interlock Weak intermolecular forces

Recent advances in phenazine-linked porous catalysts toward photo/electrocatalytic applications and mechanism

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Green Energy & Environment 2024年第10期9卷 1518-1549页

作者： Yang Liu Yu Zhang Zhao-Di Yang Liqiang Jing Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy catalytic Materials School of Material Science and Chemical EngineeringHarbin University of Science and Technology Institute of Process Engineering Chinese Academy of Sciences Key Laboratory of Functional Inorganic Materials Chemistry(Ministry of Education) School of Chemistry and Materials Science International Joint Research Center for Catalytic Technology Heilongjiang University

In recent years, porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores, high specific surface area, chemical and thermal stability, and diverse functional building blocks. Phenazine-linked organic catalysts,exhibited excellent conjugation, electrical conductivity, chemical, and thermal stability, could bring in N atoms with specific numbers and positions to regulate electron levels, anchor metals, and absorb near-infrared light, which expands solar energy utilization. These advantages of the phenazine-linked catalysts attracted our group and numerous researchers to conduct experimental and computational work on photo/electrocatalytic applications and mechanisms. This review summarizes the recent significant research progress, synthesis methods, photo/electrocatalytic performance, and applications of relative phenazine-linked catalysts. Furthermore, the photo/electrocatalytic mechanism was systematized and summarized by combining experiments and density functional theory calculations simultaneously.

关键词： Phenazine-linked porous catalysts Photo/electrocatalytic applications catalytic mechanism

Advances in sodium-ion batteries at low-temperature: Challenges and strategies

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Journal of Energy Chemistry 2024年第3期90卷 518-539,I0012页

作者： Haoran Bai Xiaohui Zhu Huaisheng Ao Guangyu He Hai Xiao Yinjuan Chen Key Laboratory of Advanced catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterChangzhou UniversityChangzhou 213164JiangsuChina Department of Chemistry Tsinghua UniversityBeijing 100084China

With the continuing boost in the demand for energy storage,there is an increasing requirement for batteries to be capable of operation in extreme environmental ***-ion batteries(SIBs) have emerged as a highly promising energy storage solution due to their promising performance over a wide range of temperatures and the abundance of sodium resources in the earth's *** to lithiumion batteries(LIBs),although sodium ions possess a larger ionic radius,they are more easily desolvated than lithium *** rthermore,SIBs have a smaller Stokes radius than lithium ions,resulting in improved sodium-ion mobility in the ***,SIBs demonstrate a significant decrease in performance at low temperatures(LT),which constrains their operation in harsh weather *** the increasing interest in SIBs,there is a notable scarcity of research focusing specifically on their mechanism under LT *** review explores recent research that considers the thermal tolerance of SIBs from an inner chemistry process perspective,spanning a wide temperature spectrum(-70 to100℃),particularly at LT *** addition,the enhancement of electrochemical performance in LT SIBs is based on improvements in reaction kinetics and cycling stability achieved through the utilization of effective electrode materials and electrolyte ***,the safety concerns associated with SIBs are addressed and effective strategies are proposed for mitigating these ***,prospects conducted to extend the environmental frontiers of commercial SIBs are discussed mainly from three viewpoints including innovations in materials,development and research of relevant theoretical mechanisms,and intelligent safety management system establishment for larger-scale energy storage SIBs.

关键词： Low-temperature Sodium-ion batteries Reaction kinetics Cycle stability Safety concerns of Sodium-ion batteries

Understanding the catalytic performance and deactivation behaviour of second-promoter doped Pt/WO_(χ)/γ-Al_(2)O_(3) catalysts in the glycerol hydrogenolysis for selective and cleaner production of 1,3-propanediol

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Journal of Energy Chemistry 2024年第7期94卷 486-507页

作者： Rafik Rajjak Shaikh Sittichai Damruang Rais Ahmad Khan Supareak Praserthdam Piyasan Praserthdam center of Excellence on Catalysis and catalytic Reaction Engineering(CECC) Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailand Department of Chemistry College of ScienceKing Saud UniversityP.O.Box 2455Riyadh 11451Saudi Arabia High-Performance Computing Unit(CECC-HCU) Centre of Excellence on Catalysis and Catalytic Reaction Engineering(CECC)Department of Chemical EngineeringFaculty of EngineeringChulalongkorn UniversityBangkok 10330Thailand

The selective aqueous-phase glycerol hydrogenolysis is a promising reaction to produce commercially useful 1,3-propanediol(1,3-PDO).The Pt-WOx bifunctional catalyst can catalyse the glycerol hydrogenol-ysis but the catalyst deactivation via sintering,metal leaching,and coking can predominantly occur in the aqueous phase *** this work,the effect of reaction temperature,pressure and second promoter(Cu,Fe,Rh,Mn,Re,Ru,Ir,Sn,B,and P)on catalytic performance and deactivation behaviour of Pt/WOx/-Al2O3 was *** doped with Rh,Mn,Re,Ru,Ir,B,and P,the second promoter boosts catalytic activity by promoting great dispersion of Pt on support and increasing Pt surface *** increased Bronsted acid sites lead to selective synthesis of 1,3-PDO than 1,2-propanediol(1,2-PDO).The characterization studies of fresh and spent catalysts reveal that the main cause of catalyst deactivation is the Pt sintering,as interpreted based on XRD,CO chemisorption,and TEM *** Pt sintering is affected depending on the second promoter that can either or reduce the interaction between Pt,WO_(χ)/γ and Al_(2)O_(3).As an electron acceptor of Pt in Pt/WO_(χ)/γ-Al_(2)O_(3),Re and Mn as second promoters resulted in increased Pt^(2+) on the catalytic surface,which strengthens the contact between Pt andγ-Al_(2)O_(3) and WO_(χ),resulting in a decrease in Pt *** metal leaching and coking are not affected by the presence of second *** catalyst modified with a second promoter possesses improved catalytic activity and 1,3-PDO production,however the stability continues to remain a *** present work unrav-elled the determining parameters of catalytic activity and deactivation,thus providing a promising pro-tocol toward effective catalysts for glycerol hydrogenolysis.

关键词： Glycerol hydrogenolysis 1,3-propanediol Metal-support interaction Second promoter Liquid phase Catalyst deactivation

Facile synthesis of hierarchical NiO/NiFe_(2)O_(4) microsphere composite as efficient visible photocatalyst for 2,4-DCP degradation

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Rare Metals 2024年第4期43卷 1580-1588页

作者： Shabana Shaheen Shuai Xu Ji Bian Amir Zada Zi-Qing Zhang Yang Qu Li-Qiang Jing Key Laboratory of Functional Inorganic Materials Chemistry(Ministry of Education) International Joint Research Center and Lab for Catalytic TechnologySchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin150080China Department of Chemistry Abdul Wali Khan UniversityMardan23200Pakistan

It is highly desired to develop efficient photocatalysts with recycling property for practical application to degrade toxic ***,nanosheet-assembled NiFe_(2)O_(4)microspheres with commendable activity are successfully synthesized by a facile solvothermal reaction with NH4F as the modifier,and their photoactivities are further improved by coupling with NiO through an in situ growth *** optimized nickel oxide(NiO)/nickel ferrite(NiFe_(2)O_(4))microsphere composite(5NiO/NFO-4)exhibits a satisfactory photocatalytic activity for 2,4-dichlorophenol(2,4-DCP)degradation under visible-light irradiation,which is attributed to its wide visible-light response,well-designed hierarchical structure and enhanced charge transfer and separation by coupling NiO as a high-level energy platform to accept ***,it is found that the NiO/NiFe_(2)O_(4)microsphere photocatalysts can be easily collected and recycled owing to the distinctive magnetic *** work provides a feasible route to rational design visible-light-driven photocatalysts with high-activity for environmental remediation and purification with good recyclability.

关键词： NiFe_(2)O_(4) microspheres NiO/Fe_(2)O_(4) composite Charge separation Visible-light photocatalysis 2 4-Dichlorophenol degradation

Towards catalytic reactions of Cu single-atom catalysts:Recent progress and future perspective

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Chinese Chemical Letters 2024年第2期35卷 197-207页

作者： Yitao Zhao Lei Tao Jiangsu Province Engineering Research center of Special Functional Textile Materials Changzhou Vocational Institute of Textile and GarmentChangzhou 213164China Jiangsu Key Laboratory of Advanced catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterSchool of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China

One of the urgent and challenging topics in diversified sustainable energy conversion is the development of high-performance,low-cost,and well durable *** single-atom catalysts(SACs)have become promising catalysts for diversified sustainable energy conversion due to their capability to maximize the utilization efficiency,acquire modulated electronic structure and optimized binding strength with *** this review,we have provided an interview of the recent progress achieved in the field of electrocatalysis,photocatalysis,and heterogeneous reaction based on Cu *** by this review,we have summarized some advanced synthetic strategies for the construction of Cu ***,the performance-improving strategies are discussed in terms of the coordination environments of the reaction center,reaction mechanism and selectivity,based on free energy diagram and electron structure ***,the remaining issues,challenges,and opportunities of Cu SACs are also provided,affording a perspective for future *** review not only offers us a deep understanding on the catalytic mechanism of Cu SACs for energy conversion,but also encourages more endeavors in prompting their practical application.

关键词： Cu SACs Energy conversion Catalysis Coordination environment

Constructing high-capacity and flexible aqueous zinc-ion batteries with air-recharging capability using organic cathodes

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Chinese Chemical Letters 2024年第3期35卷 468-472页

作者： Xiaojuan Chen Haoqi Su Baozhu Yang Xiaocen Liu Xiuting Song Lixin Su Gui Yin Qi Liu Jiangsu Key Laboratory of Advanced catalytic Materials and Technology Advanced Catalysis Green Manufacturing Collaborative Innovation Center and School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing 210093China

Flexible aqueous zinc-ion batteries(AZIBs)with air-recharging capability are a promising self-powered system applied in future wearable *** is desired to develop high-capacity air-rechargeable ***,we developed a flexible AZIB with air-recharging capability based on trinitrohexaazatrinaphthylene(TNHATN)cathode and a ZnSO_(4)*** flexible Zn//TNHATN battery exhibits high volumetric energy density(21.36 mWh/cm^3)and excellent mechanical ***,the discharged flexible Zn//TNHATN battery can be chemical self-charged via the redox reaction between TNHATN cathode and O_(2)from the *** oxidation in air for 15 h,such flexible Zn//TNHATN battery can deliver a high specific capacity of 320 mAh/g at 0.5 A/g,displaying excellent air-recharging ***,this flexible Zn//TNHATN battery also works well in chemical or/and galvanostatic charging mixed modes,showing *** work provides a new insight for designing flexible aqueous self-powered systems.

关键词： Aqueous zinc-ion battery Trinitrohexaazatrinaphthylene Organic cathode materials Flexible air-rechargeable battery Self-powered system

Surface chemical microenvironment engineering of catalysts by organic molecules for boosting electrocatalytic reaction

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Chinese Chemical Letters 2024年第8期35卷 15-24页

作者： Xianxu Chu Lu Wang Junru Li Hui Xu Henan Key Laboratory of Biomolecular Recognition and Sensing College of Chemistry and Chemical EngineeringShangqiu Normal UniversityShangqiu 476000China Key Laboratory of Advanced catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterChangzhou UniversityChangzhou 213164China

Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alytically active *** chemical microenvironment engineering via organic molecules functional-ization is a promising strategy to tune the electrocatalytic activity since it can well modify the elec-trode/electrolyte interface and alter the reaction *** this review,we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules func-tionalization,with the special focus on the organic molecule-assisted growth mechanism and unique electronic *** importantly,the applications of organic molecule functionalized catalysts in var-ious electrocatalytic reactions are also systematically summarized,along with a deep discussion on the conclusion and *** work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.

关键词： Chemical microenvironment engineering Organic molecules Electrocatalysis Functionalization Interface