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Non-noble metal-based catalysts for acetylene semihydrogenation:from thermocatalysis to sustainable catalysis

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Science China Chemistry 2023年第7期66卷 1963-1974页

作者： Lei Zhang Jin Lin Zhenpeng Liu Jian Zhang Research&Development Institute of Northwestern Polytechnical University in Shenzhen School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710129China State Key Laboratory of Solidification Processing and School of Materials Science and Engineering Northwestern Polytechnical UniversityXi’an 710072China

Selective semihydrogenation of acetylene in raw olefin streams to ethylene is a key industrial reaction to produce polymer-grade feeds for the manufacture of corresponding polymers.The currently used process in industry is the thermocatalytic acetylene semihydrogenation with pressurized hydrogen and Pd-based catalysts at relatively high temperatures.The high cost of Pd urgently desires the design of non-noble metal-based catalysts.However,non-noble metal-based catalysts commonly require much higher reaction temperatures than Pd-based catalysts because of their poor intrinsic activity.Therefore,aiming at increasing economic efficiency and sustainability,various strategies are explored for developing non-noble metal-based catalysts for thermocatalytic and green acetylene semihydrogenation processes.In this review,we systematically summarize the recent advances in catalytic technology from thermocatalysis to sustainable alternatives,as well as corresponding regulation strategies for designing high-performance non-noble metal-based catalysts.The crucial factors affecting catalytic performance are discussed,and the fundamental structure-performance correlation of catalysts is outlined.Meanwhile,we emphasize current challenging issues and future perspectives for acetylene semihydrogenation.This review will not only promote the rapid exploration of non-noble metal-based catalysts for acetylene semihydrogenation,but also advance the development of sustainable processes like electrocatalysis and photocatalysis.

关键词： acetylene semihydrogenation non-noble metal-based catalysts thermocatalysis sustainable catalysis

Advances of photothermal chemistry in photocatalysis,thermocatalysis,and synergetic photothermocatalysis for solar-to-fuel generation

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Nano Research 2022年第12期15卷 9985-10005页

作者： Minmin Gao Tianxi Zhang Ghim Wei Ho Department of Electrical and Computer Engineering National University of Singapore4 Engineering Drive 3Singapore117583Singapore Department of Chemical and Biomolecular Engineering National University of Singapore4 Engineering Drive 4Singapore117585Singapore Institute of Materials Research and Engineering Agency for ScienceTechnology and Research(A*STAR)3 Research LinkSingapore117602Singapore

The urgency of reducing pollutants and greenhouse gas emissions while maintaining fuel supply for the development of society remains one of the greatest challenges.Solar energy,a clean and sustainable energy resource,can be converted into fuels through solar-driven catalysis,and this provides an attractive solution for future energy demand.The current development of photothermal catalysis(PTC)based on the integration of solar thermal and photochemical contributions is becoming increasingly popular for full spectrum utilization.The combination of the thermochemical and photochemical processes synergistically drives the catalytic reactions efficiently under relatively mild conditions.In this review,the mechanisms of PTC are classified based on driving forces and the benefits of photothermal effects in different PTC reactions are discussed.Subsequently,the techniques for differentiating and quantifying the various effects of PTC,including experimental designs,thermometry characterization techniques,and computational studies,are summarized.Then,the major determinant properties and architectural designs for efficient photothermal catalysts are offered.Moreover,applications for fuel generation through water splitting and carbon dioxide reduction are reviewed.Finally,the current challenges and future directions of PTC are presented.This article aims to provide a comprehensive review of the current advances in PTC along with a guide for understanding the mechanisms and rational material designs to pursue solar fuel that would diversify and increase the sustainability of our energy supply.

关键词： photothermal chemistry photocatalysis thermocatalysis water splitting CO_(2)conversion solar fuel

Catalytic methane removal to mitigate its environmental effect

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中国科学：化学英文版 2023年第4期66卷 1032-1051页

作者： Chao Wang Youxun Xu Junwang Tang Department of Chemical Engineering University College LondonLondon WCIE 7JEUK

Large reserve of methane,in the form of natural gas and methane hydrate,has been discovered and it has been intensively used as a fuel,or as a building block for the chemical synthesis.However,severe environmental and climatic issues caused by the leakage of methane during the production,transportation and use of methane are overlooked.This offers incentives for the catalytic removal of methane.Nevertheless,due to the inert nature of methane molecules,the activation of methane via thermocatalysis requires harsh reaction conditions.The high reaction temperature not only increases the capital cost but also accelerates the deactivation of catalysts due to sintering and/or coking.The development of robust and stable catalysts with a low operating temperature has become the focus of the research on thermocatalytic methane oxidation.Photocatalysis,which uses the energy of photons instead of heat to drive chemical reactions under ambient conditions,offers another approach to methane removal.This review will cover the development of high-efficiency catalysts for methane combustion in both thermo-and photocatalysis.Moreover,the fundamental understanding of the active sites,surface chemistry and reaction pathway will also be discussed.Finally,the challenges facing in the catalytic removal of methane will be summarized and potential solutions will be provided.This review will be of interest to researchers in the field of heterogeneous catalysis,materials design,and chemical engineering.

关键词： methane oxidation environmental remediation thermocatalysis photocatalysis fundamental understandings

Recent advances in the catalytic production of bio-based diol 2,5-bis(hydroxymethyl)furan

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Carbon Resources Conversion 2023年第2期6卷 116-131页

作者： Wenguang Zhao Feng Wang Kangyu Zhao Xianxiang Liu Xiaoting Zhu Le Yan Yuan Yin Qiong Xu Dulin Yin National&Local Joint Engineering Laboratory for New Petro-chemical Materials and Fine Utilization of Resources Key Laboratory of the Assembly and Application of Organic Functional Molecules of Hunan ProvinceHunan Normal UniversityChangsha 410081China Department of Chemical&Biomolecular Engineering National University of Singapore4 Engineering Drive 4Singapore 117585Singapore

Biomass-derived 2,5-bis(hydroxymethyl)furan(BHMF)has received great attention and interest due to its broad application prospects in polyesters and medicine.Over the past decades,the catalytic systems including thermocatalytic,biocatalytic,electrocatalytic,and photocatalytic hydrogenation of 5-hydroxymethylfurfural(HMF)into BHMF have been developed to a great extent.To understand the present status and challenges of BHMF production,this review systematically evaluates recent findings and developments of HMF hydrogenation through various reaction systems,with an emphasis on catalyst screening,synthesis processes,and reaction mechanism.Furthermore,a few potential research trends are also proposed,in order to provide innovative ideas for further exploration of BHMF synthesis in a simpler,efficient,and economical way.

关键词： Biomass 5-Hydroxymethylfurfural 2,5-Bis(hydroxymethyl)furan Hydrogenation thermocatalysis Biocatalysis Electrocatalysis Photocatalysis

Progress of Nb-containing catalysts for carbon dioxide reduction:a minireview

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Tungsten 2022年第4期4卷 284-295页

作者： Jun-Xian Gao Wen-Jie Tian Hua-Yang Zhang School of Environment and Civil Engineering Jiangnan UniversityWuxi214122China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA5005Australia

Nb-containing catalysts have the potential to catalyze carbon dioxide(CO_(2))reduction due to their strong surface acidity and CO_(2)activation sites.Still,they have not been widely used in the development and design of catalysts due to the theoretical/cost/safety limitations.Related advances have been continuously reported in the literature,demonstrating to some extent the promise of catalytic applications of Nb-containing catalysts in this area.In this minireview,we discuss the structure-activity relationships of Nb-containing catalysts for photo-,electro-,and thermocatalytic reduction of CO_(2).The engineering strategies of Nb-containing catalysts for enhancing the conversion and selectivity of CO_(2)reduction are discussed,ranging from Nb doping,noble metal decoration,surface acidity adjustment,oxygen vacancy engineering,and heterojunction construction to Nb or Nb_(2)O_(5) particle decoration.The theoretical calculation research for the possible reaction paths and product selectivity is also discussed.Finally,the prospects for designing and optimizing Nb-containing catalysts are proposed.With a deep understanding of catalytic activity and reaction mechanism,this minireview is expected to present the optimization of the Nb-containing catalysts for efficient and highly selective CO_(2)reduction.

关键词： Niobium Carbon dioxide reduction Photocatalysis Electrocatalysis thermocatalysis

Recent advance in single-atom catalysis

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Rare Metals 2021年第4期40卷 767-789页

作者： Zeng-Xi Wei Ya-Ting Zhu Jin-Yuan Liu Zhi-Cheng Zhang Wen-Ping Hu Hui Xu Yue-Zhan Feng Jian-Min Ma School of Physics and Electronics Hunan UniversityChangsha 410082China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University and Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China School of the Environment and Safety Engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013China Key Laboratory of Materials Processing and Mold Ministry of EducationZhengzhou UniversityZhengzhou 450002China

Single-atom catalysts(SACS) have obtained a great deal of attention in many catalytic fields due to the high atom utilization efficiency and high catalytic activity.Recently,great achievements on S ACs have been made for thermocatalysis,electrocatalysis,and photocatalysis which play an important role in obtaining value-added products.However,it remains a great challenge to fabricate S ACs with high metal loading and investigate their reaction mechanisms.Therefore,it is necessary to highlight the recent development of S ACs in these fields to guide future research.In this review,we overviewed the thermocatalysis applications of SACs in CO oxidation,preferential oxidation of CO,water-gas shift reaction,methane conversion,methanol steam reforming,aqueous-phase reforming of methanol,hydrogenation of alkynes and dienes,hydrogenation of CO,and hydrogenation of substituted nitroarenes.Moreover,the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),oxygen evolution reaction(OER),CO2 reduction reaction(CO2 RR),and N2 reduction reaction(N2 RR) for photocatalytic and electrocatalytic fields were also overviewed.Lastly,the opportunities and challenges of SACs were pointed out.

关键词： Single-atom catalysts thermocatalysis Electrocatalysis Photocatalysis Catalytic activity

Polyoxometalates based compounds for green synthesis of aldehydes and ketones

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中国化学快报:英文版 2023年第8期34卷 90-101页

作者： Kejie Qin Dejin Zang Yongge Wei School of Pharmacy and Pharmaceutical Sciences&Institute of Materia Medica Shandong First Medical University&Shandong Academy of Medical SciencesNHC Key Laboratory of biotechnology drugs(Shandong Academy of Medical Sciences)Key Lab for Rare&Uncommon Diseases of Shandong ProvinceJi’nan 250117China Key Lab of Organic Optoelectronics&Molecular Engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China

Molecular oxygen within Polyoxometalates(POMs)based compounds are ideal oxidants with high atom economy and its use results in the production of water as the only byproduct.Significant progress has been made in the development of catalytic methods for aerobic alcohol oxidation to have aldehydes and ketones with POMs based compounds.They are alternative to the use of traditional hypervalent iodine catalyst systems which are with molecular oxygen as a terminal oxidant.Further,POMs based catalysts can be applied to catalytic reactions with different modes of energization such as thermocatalysis,photocatalysis and electrocatalysis.This review summarizes the frontier advances in polyoxometalates for catalytic alcohol selective oxidation in thermocatalytic,electrocatalytic,and photocatalytic applications.The three advantages of POM catalysts in terms of performance,economy,and environmental protection are highlighted.These include the use of sol-gel and electrostatic assembly methods to increase the reaction surface area,reduce the use of precious metals,and improve the stability of POMs catalysts.The field of selective alcohol oxidation is advanced.Finally,the challenges of preparing more efficient and“green”catalysts are presented.

关键词： Polyoxometalates Alcohol oxidation thermocatalysis Photocatalysis Electrocatalysis Aldehydes Ketones