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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao yifu yu Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

A perspective to ammonia-hydrogen energy industry in China

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Science China Chemistry 2024年第6期67卷 1765-1775页

作者： Baoshun Zhang Wangyang Ji Jiewei Zhu Baian Shen Menghao Lv Bin Zhang Tihu Wang yifu yu Department of Chemistry Institute of Molecular PlusSchool of ScienceTianjin UniversityTianjin300072China Tianjin University-Asia Silicon Joint Research Center of Ammonia-Hydrogen New Energy Asia Silicon(Qinghai)Co.Ltd.Xining810007China Department of Catalysis Science and Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

1 Introduction.To meet the 1.5℃ climate goal in our planet,the world is making a hard work for decarbonization[1-5].Constructing a clean energy system based on green energy is considered as the most promising way to achieve the decarbonization goals.Northwestern China owns abundant solar and wind sources and large area of deserts[6,7].

关键词： ammonia planet energy

S-scheme heterojunction construction of Fe/BiOCl/BiVO4 for enhanced photocatalytic degradation of ciprofloxacin

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Progress in Natural Science:Materials International 2024年第2期34卷 290-303页

作者： Guanlong yu Qifang Sun Yi Yang Si Chen yuannan Long yifu Li Shiyong Ge Dian Zheng School of Hydraulic and Environmental Engineering Changsha University of Science & Technology Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province School of Environmental Engineering Wuhan Textile University

With the growing problem of water pollution caused by antibiotics,the development of photocatalysts with high photogenerated carrier separation efficiency is crucial.A high-efficiency microsphere Fe/BiOCl/BiVO4with Sscheme heterojunction was synthesized by solvothermal method and its ciprofloxacin（CIP） degradation performance were investigated under visible light.XRD,FT-IR,SEM,EDS,HRTEM and XPS results show that the photocatalytic have good crystallization,morphology and the formed a microsphere.The photocatalytic performance of Fe/BiOCl/BiVO4for CIP was superior to pure BiOCl and BiVO4due to the microsphere and formed heterostructure between BiOCl and BiVO4.The influencing factors of CIP degradation by Fe/BiOCl/BiVO4were investigated,and the results showed that Fe/BiOCl/BiVO4had high degradation efficiency not only at pH 5-9,but also in the presence of inorganic Cl-,NO3-and metal ions.Under the optimal conditions,the degradation rate of CIP was up to 100% in 75 min.In addition to CIP,the Fe/BiOCl/BiVO4photocatalysts degraded other organic pollutants,such as tetracycline,oxytetracycline,chlortetracycline,ofloxacin,levofloxacin,and rhodamine B,by more than 92%.The main active species were photogenerated holes（h+） and superoxide radicals（·O2-）.In addition,possible intermediates and toxicity of intermediates were analyzed and five potential pathways for CIP degradation were proposed.

关键词： BiOCl/BiVO4 Fe3+ doping Organic pollutant Photocatalysis S-scheme heterojunction

Efficient removal of tetracycline hydrochloride through novel Fe/BiOBr/Bi_(2)WO_(6) photocatalyst prepared by dual-strategy under visible-light irradiation

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Journal of Environmental Sciences 2024年第4期138卷 46-61页

作者： Guanlong yu Kai Yang Yi Yang yifu Li Qifang Sun Peiyuan Li Wenming Wang Fengming Song Tao Ling Xuejun Peng Zhi yu Shiquan Sun School of Hydraulic and Environmental Engineering Changsha University of Science&TechnologyChangsha 410114China Key Laboratory of Dongting Lake Aquatic Eco-Environmental Control and Restoration of Hunan Province Changsha 410114China Hunan Pilot Yanghu Reclaimed Water Co. Ltd.Changsha 410208China China Railway Wuju Group the First Engineering Co. Ltd.Changsha 410117China

It is important to investigate whether combining two modification strategies has a synergistic effect on the activity of photocatalysts.In this manuscript,Fe-doped BiOBr/Bi_(2)WO_(6) heterojunctions were synthesized by a one-pot solvothermal method,and excellent photocatalytic performance was obtained for the degradation of tetracycline hydrochloride(TCH)in water without the addition of surfactant.Combining experiments and characterization,the synergistic effect between Fe ion doping and the BiOBr/Bi_(2)WO_(6) heterojunction was elucidated.The Fe/BiOBr/Bi_(2)WO_(6) composite photocatalyst had a beneficial void structure,enhanced visible light response,and could inhibit the recombination of photogenerated support well,which improved the photocatalytic activity.The presented experiments demonstrate that Fe/BiOBr/Bi_(2)WO_(6) removes 97% of TCH from aqueous solution,while pure BiOBr and Bi_(2)WO_(6) only remove 56% and 65% of TCH,respectively.Finally,the separation and transfer mechanisms of photoexcited carriers were determined in conjunction with the experimental results.This study provides a new direction for the design of efficient photocatalysts through the use of a dual co-modification strategy.

关键词： BiOBr/Bi_(2)WO_(6) Fe-doping Dual strategy Tetracycline hydrochloride Photodegradation

Manganese-Based Catalysts for Indoor Volatile Organic Compounds Degradation with Low Energy Consumption and High Efficiency

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Transactions of Tianjin University 2022年第1期28卷 53-66页

作者： Yanbo Li Shuhe Han Liping Zhang yifu yu Institute of Molecular Plus Tianjin UniversityTianjin 300072China Center for Nanoparticle Research Institute for Basic Science(IBS)SeoulRepublic of Korea

With the development of industrialization,the emission of volatile organic compounds(VOCs)to atmosphere causes serious environmental problems and the treatment of VOCs needs to consume a lot of energy.Moreover,indoor VOCs are seriously harmful to human health.Thus,there is an urgent requirement for the development of indoor VOCs treatment technologies.Catalytic degradation of VOCs,as a low energy consumption,high efficiency,and easy to achieve manner,has been widely studied in related fields.As a kind of transition metal catalyst,manganese-based catalysts have attracted a lot of attention in the catalytic degradation of VOCs because of their unique advantages including high efficiency,low cost,and excellent stability.This paper reviews the state-of-the-art progress of manganese-based catalysts for VOCs catalytic degradation.We introduce the thermocatalytic,photocatalytic and photo-thermocatalytic degradation of VOCs on manganese-based catalysts in this paper.The optimization of manganese-based catalysts by means of structural design,decorating modification and defect engineering is discussed.

关键词： VOCs degradation Manganese-based catalysts Catalysis Low energy consumption

Electrocatalytic construction of the C–N bond from the derivates of CO_(2) and N_(2)

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Science China Chemistry 2022年第2期65卷 204-206页

作者： Yanmei Huang yuting Wang Yongmeng Wu yifu yu Bin Zhang Institute of Molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Electrochemical synthesis of C-N bond-containing compounds(e.g.,urea,amino acid,amide,amine,and their derivates)from CO_(2)/N_(2)and their derivates is emerging as a promising sustainable strategy[1-7].CO_(2)and its derived products,CO,HCOOH,(COOH)_(2),etc.,could serve as carbon sources(Figure 1)[8].N_(2),making up 80%of air,is an appealing nitrogen source.However,the low solubility of N2 and the high dissociation energy for the N≡N bond limit its application.

关键词： bond Figure solubility

Recent advances in soot combustion catalysts with designed micro-structures

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Chinese Chemical Letters 2022年第4期33卷 1763-1771页

作者： Jiang Shao Xianen Lan Chaoxin Zhang Chunmei Cao yifu yu School of Chemical Engineering Zhengzhou UniversityZhengzhou 450000China Institute of Molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

With the enhancement of the people consciousness of environment protection, soot particulates(PM)elimination has drawn wide attention in recent years. Efficient after-treatment with well-designed catalysts is one of the best ways to eliminate soot particulates that come from diesel engines. Catalysts coated on the DPF(diesel particulate filter) are considered as the main factor to lower soot ignition temperature.Improvement of the structures of the catalysts is significantly important in order to achieve good catalytic performance and high stability. Based on the structures, soot combustion catalysts can be mainly divided into three types: particle-based catalysts, 3 DOM catalysts and nanoarray catalysts. This review mainly summarized recent advances in soot combustion catalysts with different designed micro-structures, each category is explained with critical assessment and several typical examples, aiming to guide the synthesis of advanced soot combustion catalysts.

关键词： Soot oxidation Nanoparticles 3DOM structures Active oxygen species Nanoarray structures

Mechanistic insight into the controlled synthesis of metal phosphide catalysts from annealing of metal oxides with sodium hypophosphite

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Nano Research 2022年第12期15卷 10134-10141页

作者： Fanpeng Chen Bohang Zhao Mengyao Sun Cuibo Liu Yanmei Shi yifu yu Bin Zhang Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin UniversityTianjin300072China

Understanding and manipulating synthetic progress for precisely controlling the components and defects of nanomaterials is an important and challenging task in materials synthesis and nanocatalysis.Metal phosphides(MPs)have been explored as cheap advanced materials in various catalytic fields.MP materials are usually synthesized through gas-solid phosphorization reaction in a trial-to-error manner,but their formation mechanism and the origin of controlled synthesis remain unclear.Here,we combine in situ thermogravimetrc analysis-mass spectrometry(TG-MS)and quasi-in situ X-ray powder diffraction(XRD)analysis to probe the transformation mechanism from metal oxides(MOs)to MPs during the phosphorization process mediated by hypophosphite.Temperature,time,and the amount of hypophosphite are revealed as the driven forces while oxophilicity and crystallinity as the impeded forces,simultaneously control the component and defect level of a series of MP(M=Ni,Co,W,Mo,and Nb).The as-obtained WO2.9/WP is proved to be an efficient Z-scheme photocatalyst for oxidative coupling of methane with the total C2+production and C2H4 selectivity in C2+products reaching 10.75 pmolg-1 and 98.25%.Our work provides a fundamental understanding of the phosphorization treatment and thereby guides a viable synthetic route to the controlled synthesis of MOx-δ,MP,MOx-δ/MP,and MP/M heterostructured materials.

关键词： phosphorization treatment metal phosphides methodology heterostructure oxygen vacancy photocatalysis

Atomically Dispersed Ru-Decorated TiO_(2) Nanosheets for Thermally Assisted Solar-Driven Nitrogen Oxidation into Nitric Oxide

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CCS Chemistry 2022年第4期4卷 1208-1216页

作者： Yanmei Huang Changhong Wang yifu yu yu yu Weichao Wang Bin Zhang Department of Chemistry Institute of Molecular PlusSchool of ScienceTianjin UniversityTianjin 300072 College of Electronic Information and Optical Engineering Nankai UniversityTianjin 300350

Thermally assisted photodriven nitrogen oxidation to nitric oxide(NO)using air as a reactant is a promising way to supersede the traditional NO synthesis industry accompanied by huge energy expenditure and greenhouse gas emission.Meanwhile,breaking the N≡N triple bond(941 kJ·mol^(−1))in nitrogen is still challenging,and the development of more efficient catalysts is necessary.Herein,Ru single atoms decorated TiO_(2) nanosheets(Ru SAs/TiO_(2))were constructed and achieved superior performance for NO photosynthesis with a product rate of 192μmol g^(−1) h^(−1) and a quantum efficiency of 0.77% at 365 nm.Both ^(15)N isotope labeling experiments and in situ near ambient pressure X-ray photoelectron spectroscopy(in situ NAP-XPS)proved the origin of NO from N_(2) photooxidation.A series of in situ characterizations and theoretical calculations unveiled the reaction pathway of nitrogen photooxidation.Breaking the O-O bond to form(N-O)2-Ru intermediates was demonstrated as the rate-determining step.Importantly,a single-atomic structure was proven to inhibit the aggregation and inactivation of Ru,leading to outstanding durability.

关键词： nitrogen oxidation Ru single atom photosynthesis reaction pathway durability

Controllable NO Release for Catheter Antibacteria from Nitrite Electroreduction over the Cu-MOF

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天津大学学报:英文版 2023年第4期29卷 275-283页

作者： Yibo Wang yutian Qin Wei Li yuting Wang Lina Zhu Meiting Zhao yifu yu Institute of Molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistryInstitute of Molecular Aggregation ScienceTianjin UniversityTianjin 300072China College of Chemistry Nankai UniversityTianjin 300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.

关键词： Heterogeneous electrocatalysis Nitrite electroreduction NO-releasing catheter Antibacterial MOF material