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Nano research 2024年第5期17卷 3752-3760页

作者： Ben Chong Baorong Xu He Li Honghui Ou Guidong Yang XJTU-Oxford Joint International research Laboratory of catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

The diffusion,adsorption/desorption behaviors of water molecules and hydrogen molecules are of great importance in heterogeneous photocatalytic hydrogen *** the study of structure-property-performance relationships,nanoconfined space provides an ideal platform to promote mass diffusion and transfer due to their extraordinary properties that are different from the bulk ***,we designed and prepared a nanoconfined CdS@SiO_(2)-NH_(2) nanoreactor,whose shell is composed of amino-functionalized silica nanochannels,and encapsulates spherical CdS as a photocatalyst *** and simulated results reveal that the amino-functionalized nanochannels promote water molecules’and hydrogen molecules’directional diffusion and *** molecules are enriched in the nanocavity between the core and the shell,and promote the interfacial photocatalytic *** a result,the maximized water enrichment and minimized hydrogen-occupied active sites enable photocatalyst with optimized mass transfer kinetics and localization electron distribution on the CdS surface,leading to superior hydrogen production performance with activity as high as 37.1 mmol·g^(-1)·h^(-1).

关键词： nanochannels photocatalytic hydrogen evolution mass transfer amino-functionalized CdS

Tuning interaction strength between CeO_(2) and iridium to promote CO oxidation over Ir/TiO_(2)

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Journal of Rare Earths 2024年第4期42卷 651-659页

作者： Lu Dai Binghua Li Yuhan Peng Xianwei Hao Runquan Xuan Hua Huang Yiming Bi Liping Xu Yanhui Zhang Yun Guo Fangqi Du Li Wang Hui Wang technology Center China Tobacco Zhejiang Industrial Co.Ltd.Hangzhou310024China research Institute of Industrial catalysis East China University of Science and TechnologyShanghai200237China

The interaction between support and noble metal plays a crucial role in heterogeneous catalysis ***,how to tune metal support interactions to optimize the activity still needs further ***_(2) was introduced to promote CO oxidation ove r Ir/TiO_(2) by adjusting the interaction strength between iridium(Ir)and CeO_(2).The strong interaction between Ir and CeO_(2) blocks CO adsorption and causes low CO oxidation ***,introducing CeO_(2) on Ir/TiO_(2) produces localized interaction between Ir and CeO_(2),which can tune the surface electronic state of Ir,so a"volcano curve"relationship between CO oxidation activity and electronic state is *** amount of CeO_(2) on Ir/TiO_(2)(Ir/Ce_(0.2)Ti)leads to CO complete oxidization at 22℃,and a new pathway for CO oxidation was *** study demonstrates that the utilization of tuning interaction strength between active metal and support is a potential method to increase the catalytic activity.

关键词： CO oxidation CeO_(2) Localized interaction Interaction strength Supported Ir catalysts Rareearths

Combinations of electron and proton donors in transition-metal complex mediated nitrogen reduction reactions

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Science China Chemistry 2024年第7期67卷 2136-2154页

作者： Delong Han Li Yang Hao Huang Priyanka Chakraborty Shashikant U.Dighe Kuo-Wei Huang KAUST catalysis Center and Division of Physical Science and Engineering King Abdullah University of Science and TechnologyThuwal 23955Saudi Arabia Agency for Science Technologyand ResearchInstitute of Materials Research and Engineering and Institute of Sustainability for ChemicalsEnergy and EnvironmentSingapore 138634Singapore

Nitrogen fixation is a complex process involving the transfer of six electrons and *** from the conventional Haber-Bosch process,which relies on hydrogen(H_(2))to provide both electrons and protons to reduce nitrogen(N_(2)),homogeneous transition metal complex-catalyzed N_(2)reduction reactions(NRR)employ an array of electron and proton donors or even electron donors combined with *** the synthesis of diverse catalytic progress,the categories of donors have seen rapid ***,existing literature only provides summaries regarding the metal,ligands,and *** the significance of electron and proton donor combinations in nitrogen reduction reactions,no literature has thoroughly reviewed this ***,we hereby compiled a comprehensive list of commonly used reagents in N_(2)reduction and classified them according to their specific donor *** review presents clear and organized information about these combinations,along with a summary of their general performance trend in NRR with related ***,we conclude the discussion by highlighting key points for researchers to consider when selecting catalysts and donor combinations,with the ultimate goal of advancing the field of nitrogen fixation.

关键词： dinitrogen reduction reaction reducing donor combination transition metal complexes homogeneous catalysis

Efficient upcycling of high-density polyethylene into separable cyclic hydrocarbons

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Science China Chemistry 2024年第4期67卷 1049-1050页

作者： Shenglu Lu Yanqin Wang State key laboratory of green chemical engineering and industrial catalysis Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

This highlight is inspired by a recent article in Nature Nanotechnology in which Zeng and co-workers[1]from the University of Science and technology of China reported a strategy for upcycling high-density polyethylene(HDPE)into separable cyclic hydrocarbons under solvent-and hydrogen-free *** work made a significant progress in plastic recycling.

关键词： hydrocarbons cycling high

Insight into Lithium–sulfur batteries performance enhancement: from metal nanoparticles to metal nanoclusters to single metal atoms

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Tungsten 2024年第3期6卷 504-521页

作者： Shuang Ma Qing-Ling Ruan Xue-Cheng Liu Gui-Jun Zhu Die Yuan Ling-Qiao Hu Yu-Mei Huang Xing-Xing Gu Chongqing Key Laboratory of catalysis and New Environmental Materials College of Environment and Resources Chongqing Technology and Business University National research Base of Intelligent Manufacturing Service Chongqing Technology and Business University

Lithium-sulfur(Li-S) batteries have attracted much attention and developed rapidly in recent years due to their high energy density,low cost,and ***,its commercialization process still encounters various *** them,the sulfur cathode is easy to dissolve and shuttle,resulting in the loss of active substances and the severe growth of lithium anode dendrites,which is one of the biggest *** the redox conversion kinetics of sulfur cathode is expected to fundamentally alleviate the shuttle phenomenon of poly ***,this paper reviews the effects of metal nanoparticles to metal nanoclusters to metal single-atom catalysts on improving the redox of Li-S batteries,to let researchers better understand the size effect on the kinetics of sulfur cathodes in Li-S batteries,which will provide important guidance for the future large-scale commercialization of Li-S batteries.

关键词： Lithium–sulfur batteries Metal nanoparticles Metal nanoclusters Metal single atoms Size effects

Rapid Energy Exchange between In Situ Formed Bromine Vacancies and CO_(2)Molecules Enhances CO_(2)Photoreduction

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research 2024年第2期2023卷 763-771页

作者： Qin Ren Ye He Hong Wang Yanjuan Sun Fan Dong research Center for Environmental and Energy catalysis Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China School of Resources and Environment University of Electronic Science and Technology of ChinaChengdu 611731China

Photocatalytic reduction of CO_(2)into fuels provides a prospective tactic for regulating the global carbon balance utilizing renewable solar ***,CO_(2)molecules are difficult to activate and reduce due to the thermodynamic stability and chemical *** this work,we develop a novel strategy to promote the adsorption and activation of CO_(2)molecules via the rapid energy exchange between the photoinduced Br vacancies and CO_(2)*** in situ continuous wave-electron paramagnetic resonance(cw-EPR)and pulsed EPR technologies,we observe that the spin-spin relaxation time(T_(2))of BiOBr is decreased by 198 ns during the CO_(2)photoreduction reaction,which is further confirmed by the broadened EPR *** result reveals that there is an energy exchange interaction between in situ formed Br vacancies and CO_(2)molecules,which promotes the formation of high-energy CO_(2)molecules to facilitate the subsequent reduction *** addition,theoretical calculations indicate that the bended CO_(2)adsorption configuration on the surface of BiOBr with Br vacancies caused the decrease of the lowest unoccupied molecular orbital of the CO_(2)molecule,which makes it easier for CO_(2)molecules to acquire electrons and get *** situ diffuse reflectance infrared Fourier transform spectroscopy further shows that the activated CO_(2)molecules are favorably converted to key intermediates of COOH*,resulting in a CO generation rate of 9.1μmol g^(-1)h^(-1)and a selectivity of 100%.This study elucidates the underlying mechanism of CO_(2)activation at active sites and deepens the understanding of CO_(2)photoreduction reaction.

关键词： reaction. adsorption activation

Highly efficient photo-thermal synergistic catalysis of CO_(2)methanation over La_(1-x)Ce_(x)NiO_(3)perovskite-catalyst

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Nano research 2024年第9期17卷 7945-7956页

作者： Ting Li Zhen-Yu Zhang De-Cun Luo Bo-Yu Xu Rong-Jiang Zhang Ji-Long Yao Dan Li Tao Xie Institute of Industrial catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

Solar-driven photo-thermal catalytic CO_(2)methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases ***,designing advanced photo-thermal catalysts remains a research challenge for CO_(2)methanation *** this work,a series of ABO3(A=lanthanide,B=transition metal)perovskite catalysts with Ce-substituted LaNiO3(La_(1-x)Ce_(x)NiO_(3),x=0,0.2,0.5,0.8,1)were synthesized for CO_(2)*** La_(0.2)Ce_(0.8)NiO_(3) exhibited the highest CH_(4) formation rate of 258.9 mmol·g^(-1)·hcat-1,CO_(2)conversion of 55.4%and 97.2%CH_(4) selectivity at 300℃with the light intensity of 2.9 W·cm^(-2).Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties *** partial substitution of the A-site provided more active sites for the adsorption and activation of CO_(2)/H_(2).The sources of the active sites were considered to be the oxygen vacancies(O_(v))created by lattice distortions due to different species of ions(La^(3+),Ce^(4+),Ce^(3+))and exsolved Ni0 by H_(2)*** catalysts have excellent light absorption absorbance and low electron-hole(e^(-)/h^(+))recombination rate,which greatly contribute to the excellent performance in photo-thermal synergistic catalysis(PTC)CO_(2)*** results of in situ irradiated electron paramagnetic resonance spectrometer(ISI-EPR)and ISI-X-ray photoelectron spectroscopy(XPS)indicated that the aggregation of unpaired electrons near the defects and Ni metal(from La and Ce ions to Ov and Ni0)accelerated adsorption and activation of CO_(2)/H_(2).At last,the catalyst properties and structure were correlated with the proposed reaction mechanism from the in situ diffuse reflection infrared Fourier transform spectrum(DRIFTS)*** in situ precipitation of the B-site enhanced the dispersion of Ni,while its enriched photoelectrons upon illumination further promote hydrogen *** H^(*)spillover accelerated t

关键词： photo-thermal catalysis CO_(2)methanation perovskite A-site substitution in situ diffuse reflection infrared Fourier transform spectrum(DRIFTS)

Photodegradation of xylene isomers:Kinetics,mechanism,secondary pollutant formation potential and health risk evaluation

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Journal of Environmental Sciences 2024年第2期136卷 658-669页

作者： Xiaoyan Chen Weikun Zhu Sufen Feng Jiangyao Chen Guangdong Key Laboratory of Environmental catalysis and Health Risk Control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental catalysis and Pollution Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Photodegradation technology has been widely applied in the purification of industrial aromatic ***,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still ***,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light *** lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 *** xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and *** them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of ***,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure ***,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded *** findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.

关键词： Isomer aromatics Photodegradation Ozone formation Secondary organic aerosols Health risk

Rational design and energy catalytic application of high-loading single-atom catalysts

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Rare Metals 2024年第10期43卷 4844-4866页

作者： Zi-Wei Deng Yue Liu Jie Lin Wen-Xing Chen Energy and catalysis Center School of Materials Science and EngineeringBeijing Institute of Technology Ningbo Institute of Materials technology and Engineering Chinese Academy of Science

It is well known that single-atom catalysts(SACs)have become a hot topic in the field of catalysis due to their advantages such as 100% metal atom utilization efficiency,high catalytic activity and selectivity compared with conventional catalysts and nanocatalysts. However, the isolated metal atoms on SACs have thermodynamic instability and tend to agglomerate, which limit their catalytic ***, it is of great significance to synthesize stable and high-loading single-atom catalysts(HLSACs). In this paper,we review the research progress of HLSACs from two aspects:design and application. Firstly, we comprehensively introduce the synthesis strategies of HLSACs, namely, top-down and bottom-up methods. Secondly, we overview the application status of HLSACs in three fields: electrocatalysis, thermal catalysis and photocatalysis. Finally, we summarize the development prospects and challenges of HLSACs.

关键词： Design Electrocatalysis High-loading single-atom catalysts Photocatalysis Thermal catalysis

Design and synthesis of polyoxovanadate-based framework for efficient dye degradation

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Tungsten 2024年第2期6卷 447-453页

作者： Qing Lan Su-Juan Jin Zheng Wang Xu-Yang Li Yan Xiong Zhuo-Cheng Wang Shan-Shan Liu Zhi-Ming Zhang Qiang Zhao Engineering technology research Center of Henan Province for Solar catalysis School of Chemical and Pharmaceutical EngineeringNanyang Normal UniversityNanyang 473061China Institute of New Energy Materials&Low Carbon technology Tianjin University of TechnologyTianjin 300384China

A new polyoxovanadate-based framework material[Cu(en)_(2)]_(4)V_(18)O_(42)(H_(2)O)·6H_(2)O(1)was designed and synthesized by hydrothermal reaction of NaVO_(3),Cu(NO_(3))_(2)·6H_(2)O and 1,2-diaminoethane(en)via carefully adjusting the pH value of the reaction *** structure of the title compound has been determined by single-crystal X-ray diff raction analysis,thermogravimetric analysis,infrared spectra and elemental *** structural analysis demonstrate the three-dimensional(3D)framework structure of compound 1,which was composed of the[V_(18)O_(42)(H_(2)O)]_(8)−({V_(18)O_(42)(H_(2)O)})anions linked by the Cu^(2+)*** 1 represents the fi rst 3D framework based on{V_(18)O_(42)(H_(2)O)}polyoxoanions and copper ***-driven degradation of residual organic pollutants in industrial wastewater is still a major problem for human *** experiments reveal that compound 1 possesses of excellent photocatalytic activity for the degradation of methylene blue and rhodamine B.

关键词： Polyoxovanadate Framework Polyoxovanadate-based framework Photocatalytic Organic pollutants