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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)

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Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of Environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao institute of catalysis for Energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high *** study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) *** further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and ***,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate *** H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/*** calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational ***,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) *** indicted that the chemisorptions of aldehyde oxygen have largest *** results suggested adsorption conformations have a respectable impact on the catalysis *** study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

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Single-atom catalysis:a promising avenue for precisely controlling reaction pathways

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Frontiers of Chemical Science and Engineering 2024年第7期18卷 97-120页

作者： Xiaobo Yang Xuning Li Yanqiang Huang State Key Laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Single-atom catalysts (SACs), characterized by exceptionally high atom efficiency, have garnered significant attention across various catalytic reactions. Recent studies have showcased SACs with robust capabilities for precise catalysis, specifically targeting reactions along designated pathways. This review focuses on the advances in the precise activation and reconstruction of chemical bonds on SACs, including precise activation of C–O and C–H bonds and selective couplings involving C–C and C–N bonds. Our discussion begins with a thorough exploration of the factors that render SACs skilled in precise catalytic processes, encompassing the narrow d-band electronic state of single atom site resulting in the adsorption tendency, isolate site resulting in unique adsorption structure, and synergy effect of a single atom site with its neighbors. Subsequently, we elaborate on the applications of SACs in electrocatalysis and thermocatalysis including four prominent reactions, namely, electrochemical CO_(2) reduction, urea electrochemical synthesis, CO_(2) hydrogenation, and CH4 activation. Then the concept of rational design of SACs for precisely controlling reaction pathways is discussed from the aspects of pore structure design, support-metal strong interaction, and support hydrophilic/hydrophobic. Finally, we summarize the challenges encountered by SACs in the field of precise catalytic processes and outline prospects for their further development in this domain.

关键词： single atom catalysts selective oxidation CO_(2)RR bond coupling

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Metal-N_(4)model single‐atom catalyst with electroneutral quadri‐pyridine macrocyclic ligand for CO_(2)electroreduction

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Carbon Energy 2024年第8期6卷 122-133页

作者： Jian‐Zhao Peng Yin‐Long Li Yao‐Ti Cheng Fu‐Zhi Li Bo Cao Qing Wang Xian Yue Guo‐Tao Lai Yang‐Gang Wang Jun Gu Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdongChina institute for catalysis Hokkaido UniversitySapporoJapan

Metal–N–C single‐atom catalysts,mostly prepared from pyrolysis of metalorganic precursors,are widely used in heterogeneous *** metal sites with diverse local structures coexist in this type of material and it is challenging to characterize the local structure,a reliable structure–property relationship is difficult to *** macrocyclic complexes adsorbed on carbon support are well‐defined models to mimic the singleatom ***–N_(4)site with four electroneutral pyridine‐type ligands embedded in a graphene layer is the most commonly proposed structure of the active site of single‐atom catalysts,but its molecular counterpart has not been *** this work,we synthesized the conjugated macrocyclic complexes with a metal center(Co,Fe,or Ni)coordinated with four electroneutral pyridinic ligands as model catalysts for CO_(2)*** comparison,the complexes with anionic quadri‐pyridine macrocyclic ligand were also *** Co complex with the electroneutral ligand expressed a turnover frequency of CO formation more than an order of magnitude higher than that of the Co complex with the anionic *** ab initio molecular dynamics simulations based on the well‐defined structures of the model catalysts indicate that the Co complex with the electroneutral ligand possesses a stronger ability to mediate electron transfer from carbon to CO_(2).

关键词： ab initio molecular dynamics CO_(2)reduction electrocatalysis model catalyst single‐atom catalyst

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Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient oxidative self-coupling of benzylamines

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Frontiers of Chemical Science and Engineering 2024年第1期18卷 95-106页

作者： Jie Chen Mingyuan Jian Deqiong Xie Kecan Dou Deli Chen Weidong Zhu Fumin Zhang Key Laboratory of the Ministry of Education for Advanced catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

In this study,we synthesize a catalyst comprising cobalt nanoparticles supported on MXene by pyrolyzing a composite in a N2 ***,the composite comprises a bimetallic Zn/Co zeolitic imidazole framework grown in situ on the outer surface of *** catalytic efficiency of the catalyst is tested for the self-coupling of 4-methoxybenzylamine to produce value-added imine,where atmospheric oxygen(1 atm)is used as the *** on the results,the catalyst displayed impressive catalytic activity,achieving 95.4%yield of the desired imine at 383 K for 8 ***,the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional *** outstanding performance of the catalyst is primarily attributed to the synergetic catalytic effect between the cobalt nanoparticles and MXene support,while also benefiting from the three-dimensional porous ***,a preliminary investigation of potential reaction mechanisms is conducted.

关键词： MXene sacrificial template oxidative self-coupling Co nanoparticles imine

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Cu/TiO_(2) Photocatalysts for CO_(2) Reduction: Structure and Evolution of the Cocatalyst Active Form

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Transactions of Tianjin University 2024年第2期30卷 140-151页

作者： Andrey A.Saraev Anna Yu.Kurenkova Denis D.Mishchenko Alexandr L.Trigub Evgeniy Yu.Gerasimov Ekaterina A.Kozlova Boreskov institute of catalysis Lavrentieva Ave 5Novosibirsk 630090Russia Synchrotron Radiation Facility SKIF Boreskov Institute of CatalysisNikol’skiy Ave 1Kol’tsovo 630559Russia National Research Center “Kurchatov Institute”Kurchatova Sq 1Moscow 123182Russia

Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spectroscopy, high-resolution transmis- sion electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. It was found that copper exists in different states (Cu 0 , Cu^(+) , and Cu^(2+) ), the content of which depends on the TiO_(2) calcination temperature and copper loading. The optimum composition of the cocatalyst has a photocatalyst based on TiO_(2) calcined at 700℃ and modified with 5 wt% copper, the activity of which is 22 μmol/(h·g cat ) (409 nm). Analysis of the photocatalysts after the photocatalytic reaction disclosed that the copper metal on the surface of the calcined TiO_(2) was gradually converted into Cu_(2) O during the photocatalytic reaction. Meanwhile, the metallic copper on the surface of the noncalcined TiO_(2) did not undergo any trans- formation during the reaction.

关键词： Photocatalysis Photocatalytic CO_(2)conversion Visible light Titanium dioxide Copper Copper oxides Methane formation Photocatalyst transformation

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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

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Revisiting the sodium-ion storage capability of hard carbon in carbonate-based electrolytes via a sodium-metal-free protocol

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Science China Chemistry 2024年第7期67卷 2240-2247页

作者： Gaopan Liu Yanbing Mo Jiawei Chen Yu Peng Xiao Zhu Fei Wang Xiaoli Dong Yongyao Xia Department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and Innovative Materials Institute of New EnergyLaboratory of Advanced MaterialsFudan UniversityShanghai 200438China

Common evaluation methodology of sodium(Na)-containing two-electrode or three-electrode configurations overlooks the interference from highly reactive Na metal,leading to the underestimation or inconsistent performance of low-potential hard carbon(HC)***,the trap of Na metal was systematically investigated with or without applied current,uncovering its inadequacy as the reference or counter electrode in different configurations.A Na-metal-free three-electrode protocol is proposed for evaluating the actual Na^(+)-storage capability of the typical low-potential HC *** avoiding Na crosstalk and precisely controlling the working electrode's potential,the actual electrochemical performance of HC in the carbonate esterbased electrolyte can be recognized with high capacity of 222 mAh g^(-1)at 2 C and 113 mAh g^(-1)at 5 C,correcting the misunderstanding of the inferior performance of HC in coin-type half cells(68%and 50%undervaluation at 2 C and 5 C,respectively).The advanced protocol is expected to reduce misunderstandings or underestimation due to evaluation methods and to guide the development of high-performance battery materials.

关键词： highly reactive sodium potential drift carbonate ester sodium-metal-free protocol sodium storage capability

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Effect of valence and spin state on ethane dehydrogenation in Fe-S-1 catalyst

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Journal of Energy Chemistry 2024年第10期97卷 677-686页

作者： Liusai Huang Yumeng Fo Peng Zhang Shaojia Song Xinxin Zhang Xueqiu Wu Saeed Soltanali Jian Liu Weiyu Song State Key Laboratory of Heavy Oil Processing China University of Petroleum (Beijing) China Petrochemical Research institute PetroChina Company Limited catalysis Technologies Development Division Research Institute of Petroleum Industry (RIPI)

Light alkanes non-oxidative dehydrogenation is an attractive non-oil route for olefins *** alkane dehydrogenation reaction is limited by thermodynamic equilibrium,and the C-H bond cleavage is commonly considered as the rate-determined *** valence state of metal sites in catalysts will influence the stabilization of the vital intermediate(i.e.,CxHy...Mδ+...H) during the C-H bond cleavage process,which in turn affects the catalytic ***,we explicitly investigated the effect of different valence states of framework-Fe in silicate-1 zeolite on ethane dehydrogenation reaction through the combination of experimental and theoretical ***（Ⅱ）-S-1 and Fe（Ⅲ）-S-1 catalysts are successfully synthesized by ligand-assisted in situ crystallization method,In-situ C2H6-FTIR shows the higher coverage of hydrocarbon intermediates on Fe（Ⅱ）-S-1,Under the same evaluation co nditio n,Fe（Ⅱ）-S-1 exhibits a higher space time yield of *** functional theory（DFT） results reveal that the more coordinate-unsaturated and electron-enriched Fe（Ⅱ） sites boost the first C-H bond activation by slight deformation and efficient electron donation with C2H5****,the second C-H bond cleavage on Fe（Ⅱ）-S-1 undergoes a spin-crossing process from quintet state to triplet state,which involves a two-electro n-two-orbital interaction,further promoting the formation of *** analysis is consistent with the experimental and DFT *** work could provide methodology for elucidating the effect of metal valence states on catalytic performance as well as offer guidance for designing more efficient Fe-zeolite catalysts.

关键词： DFT Electron-enriched Ethane dehydrogenation Iron Spin crossover

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Catalyst design and structure control for photocatalytic refineries of cellulosic biomass to fuels and chemicals

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Journal of Energy Chemistry 2024年第7期94卷 102-127页

作者： Lulu Sun Nengchao Luo State Key Laboratory of catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Lignocellulosic biomass is the largest renewable hydrocarbon resource on *** cellulose,one of the major components of lignocellulose,powered by solar energy is a promising way of providing lowcarbon-footprint energy chemicals such as H_(2),HCOOH,CO,and transportation ***-of-the-art biorefineries target the full use of biomass feedstocks as they have a maximum collection radius of 75-100 km,requesting efficient and selective photocatalysts that significantly influence the outcome of photocatalytic ***-performed photocatalysts can harvest a broad solar spectrum and are active in breaking the chemical bonds of cellulose,decreasing the capital investments of ***,photocatalysts should control the selectivity of cellulose conversion,originating target products to level down separation *** separation in photocatalysts and interfacial charge transfer between photocatalysts and cellulose affect the activity and selectivity of cellulose refineries to H2 and carbonaceous *** account for the challenges above,this review summarizes photocatalysts for the refineries of cellulose and downstream platform molecules based on the types of products,with the structure features of different types of photocatalysts discussed in relation to the targets of either improving the activity or product *** addition,this review also sheds light on the methods for designing and regulating photocatalyst structures to facilitate photocatalytic refineries of cellulose and platform molecules,meanwhile summarizing proposed future research challenges and opportunities for designing efficient photocatalysts.

关键词： Photocatalysts Biorefineries Cellulose Fuels Hydrogen

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