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Science China Chemistry 2024年第7期67卷 2206-2214页

作者： Menglin Xie Ting Li Chao Wu Xiaoling Liu Jinling Ni Siqin Yao Yu Zhou Shibo Xi Jun Wang State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Institute of Sustainability for Chemicals Energy and Environment(ISCE2)Agency for ScienceTechnology and Research(A*STAR)Singapore 627833Republic of Singapore College of Materials Science and Engineering Sichuan UniversityChengdu 610065China

The selective oxidation of cyclohexane is a promising green route for the production of KA oil(cyclohexanol and cyclohexanone),but remains a huge challenge to design high-performing heterogeneous catalysts under mild ***,a pure silica ZSM-12(MTW topology)zeolite was applied as the support to immobilize highly dispersive tetrahedrally coordinated vanadium(V)species and the constructed catalyst 1%V/SZ-12 exhibited high efficiency in the fast and selective oxidation of cyclohexane into cyclohexanone with H_(2)O_(2).The reaction completed within 30 s,affording the selectivity of 99%towards cyclohexanone and the extremely high turnover frequency(TOF)of 5,891 h^(-1).1%V/SZ-12 was facilely reused with stable activity and feasibly extended to the oxidation of various cyclohexane *** one-dimensional 12-membered ring microchannels contributed to the formation and accessibility of tetrahedrally coordinated high valent V5+species as the robust active centers,which activated H_(2)O_(2) to generate V–O–O·,the active oxygen species for the electrophilic attack on cyclohexane to produce cyclohexanone as the sole product.

关键词： zeolite metal doping cyclohexane oxidation heterogeneous catalysis

Integrated CO_(2)capture and reduction catalysis:Role ofγ-Al_(2)O_(3)support,unique state of potassium and synergy with copper

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Journal of Environmental Sciences 2024年第6期140卷 113-122页

作者： Donato Pinto Stefano Minorello Zhouping Zhou Atsushi Urakawa catalysis Engineering Department of Chemical EngineeringDelft University of TechnologyDelft2629HZNetherlands

Carbon dioxide capture and reduction(CCR)process emerges as an efficient catalytic strategy for CO_(2)capture and conversion to valuable chemicals.K-promoted Cu/Al_(2)O_(3)catalysts exhibited promising CO_(2)capture efficiency and highly selective conversion to syngas(CO+H_(2)).The dynamic nature of the Cu-K system at reaction conditions complicates the identification of the catalytically active phase and surface *** present work aims at more precise understanding of the roles of the potassium and copper and the contribution of the metal oxide ***γ-Al_(2)O_(3)guarantees high dispersion and destabilisation of the potassium phase,potassium and copper act synergistically to remove CO_(2)from diluted streams and promote fast regeneration of the active phase for CO_(2)capture releasing CO while passing H_(2).A temperature of 350℃is found necessary to activate H_(2)dissociation and generate the active sites for CO_(2)*** effects of synthesis parameters on the CCR activity are also described by combination of ex-situ characterisation of the materials and catalytic testing.

关键词： Carbon dioxide Carbon capture and utilisation CO_(2)capture and reduction Solid CO_(2)sorbents heterogeneous catalysis Potassium Copper catalysts Aluminium oxide

Advances of graphdiyne-supported metal catalysts in thermocatalytic reactions

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Nano Research 2024年第4期17卷 2223-2233页

作者： Jia Yu Yida Yang Yuliang Li Changyan Cao Weiguo Song Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of Molecular Nanostructures and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of organic solidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Supported metal catalysts are widely used in the modern chemical *** electronic interaction between supports and active components is of great significance for heterogeneous ***(GDY),a new type of carbon allotrope with sp-hybridized carbon atoms,πconjugate structure,and electron transmission capability,is a promising candidate as catalyst *** years have witnessed the rapid progress of GDY-supported metal catalysts for different catalysis *** that most processes in the current chemical industry are thermocatalytic reactions,we herein give an overview about the advances and particular characteristics of GDY-supported catalysts in these *** geometric structure and electronic properties of GDY are first ***,the synthesis methods for GDY-supported metal catalysts and their applications in thermocatalytic reactions are discussed,in which the effect of electronic interaction on catalytic performance is ***,the current challenges and future directions of GDY-supported metal catalysts for thermocatalysis are *** is expected that this review will enrich our understanding of the advances of GDY as a superior support for metal catalysts in thermocatalytic reactions.

关键词： graphdiyne metal catalysts thermocatalytic reactions heterogeneous catalysis

Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

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Journal of Energy Chemistry 2024年第5期92卷 16-25页

作者： Baoyu Wang Jinshu Huang Hongguo Wu Ximing Yan Yuhe Liao Hu Li National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCollege of Pharmacy&Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Guangxi Key Laboratory of Green Chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of ***,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous *** synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical ***,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer *** in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

关键词： Biomass conversion heterogeneous catalysis Lignin Dual-atom catalyst Selective C-ocleavage

Surface/Interface Engineering of Hierarchical MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterogeneous Nanosheet Arrays for Alkaline Water Electrolysis with Fast Kinetics

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Chinese Journal of Chemistry 2024年第2期42卷 119-128页

作者： Qiong Zhang Ruixue Zhang Yingxiu Zhao Tiantian Sun Jianyang Gao Guang-Rui Xu Zexing Wu Yu Yang Lei Wang Key Laboratory of Eco-chemical Engineering Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life ScienceTaishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyCollege of Chemistry and Molecular EngineeringSchool of Materials Science and EngineeringQingdao University of Science and TechnologyQingdaoShandong 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdaoShandong 266042China

Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water ***,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of *** from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)*** synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water ***,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline *** building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.

关键词： Hierarchical heterostructure Surface engineering Bifunctional catalysts Hydrogen evolution reaction Oxygen evolution reaction Watersplitting Catalytic activity Electrocatalysis heterogeneous catalysis

Recent advances in heterogeneous hydrosilylation of unsaturated carbon-carbon bonds

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Chinese Chemical Letters 2024年第6期35卷 71-85页

作者： Heng Yang Zhijie Zhou Conghui Tang Feng Chen School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The hydrosilylation of unsaturated carbon-carbon bonds is one of the most critical reactions in silicone industrial *** homogeneous Speier's catalyst,Karstedt's catalyst,and other noble metal-based catalysts are widely ***,simplifying the separation of the homogeneous catalyst from reaction products and reducing the high cost of precious metals is still *** review describes the recent development of heterogeneous catalysts for alkene,alkyne,and allene hydrosilylations,which can effectively solve problems in homogeneous hydrosilylation.

关键词： Hydrosilylation heterogeneous catalysis Alkenes Alkynes Silanes

Anisotropic Plasmon Resonance Enables Spatially Controlled Photothermal and Photochemical Effects in Hot Carrier-Driven catalysis

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Chinese Journal of Chemistry 2024年第16期42卷 1877-1885页

作者： Jiaqi Wang Zhijie Zhu Kai Feng Shuang Liu Yuxuan Zhou Ifra Urooj Jiari He Zhiyi Wu Jiahui Shen Xu Hu Zhijie Chen Xudong Dong Manzar Sohail Yanyun Ma Jinxing Chen Chaoran Li Xingda An Le He Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhouJiangsu 215123China Jiangsu Key Laboratory ofAdvanced Negative Carbon Technologies Soochow UniversitySuzhouJiangsu 215123China Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices Soochow UniversitySuzhouJiangsu 215123China Department of Chemistry School of Natural SciencesNational University of Sciences and TechnologyIslamabad 44000Pakistan

Localized surface plasmon resonance has been demonstrated to provide effective photophysical enhancement mechanisms in plasmonic ***,it remains highly challenging for distinct mechanisms to function in synergy for a collective gain in catalysis due to the lack of spatiotemporal control of their ***,the anisotropic plasmon resonance nature of Au nanorods was exploited to achieve distinct functionality towards synergistic *** and photochemical effects were enabled by the longitudinal and transverse plasmon resonance modes,respectively,and were enhanced by partial coating of silica nanoshells and epitaxial growth of a reactor *** excitation leads to a synergistic gain in photothermal-mediated hot carrier-driven hydrogen evolution *** approach provides important design principles for plasmonic photocatalysts in achieving spatiotemporal modulation of distinct photophysical enhancement *** also effectively broadens the sunlight response range and increases the efficacy of distinct plasmonic enhancement pathways towards solar energy harvesting and conversion.

关键词： Plasmon resonance Photothermal effect Photochemistry Photocatalysis Metal nanoparticles Charge carrier injection heterogeneous catalysis Photoelectrochemistry

Selective N-Methylation of N-Methylaniline with CO_(2) and H_(2) over Cu/In_(2)O_(3) Catalyst

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Chinese Journal of Chemistry 2024年第3期42卷 276-282页

作者： Huan Zheng Bo Qian Lin He State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouGansu730000 China University of Chinese Academy of Sciences Beijing100049 China

N-Methylation of amines with CO_(2) and H2 is a potential approach for CO_(2) utilization because N-methylated amines can be used as solvents and organic intermediates. In_(2)O_(3)-supported Cu (Cu/In_(2)O_(3)) acts as an effective heterogeneous catalyst for N-methylation reaction of N-methylaniline (MA) with CO_(2) and H_(2),showing higher N,N-dimethylaniline (DMA) selectivity than other supported Cu catalysts. On one hand,the dispersion of Cu can be improved by the defective In_(2)O_(3) support. On the other hand,In_(2)O_(3) support is active in the dissociative adsorption of CO_(2) through C—O bond breaking. In addition,the H_(2) dissociation ability of In_(2)O_(3) can also be enhanced by Cu. The combination of Cu and In_(2)O_(3) is effective in the activation of CO_(2),the adsorption of intermediate N-methylformanilide (MFA),the hydrogenation of MFA to DMA and the prohibition of C—N bond cleavage side reactions,thereby enhancing the reaction rate of MA conversion and the selectivity to DMA.

关键词： N-Methylation CO_(2) Cu/In_(2)O_(3) Supported catalysts heterogeneous catalysis

Exploration of Strong Metal-Support Interaction in heterogeneous Catalysts by in situ Transmission Electron Microscopy

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Chinese Journal of Chemistry 2024年第9期42卷 1004-1008页

作者： Yongjun Jiang Sheng Dai Key Laboratoryfor Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool of Chemistry&Molecular EngineeringEast China Universityof Science and TechnologyShanghai 200237China

The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous ***,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI *** emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.

关键词： heterogeneous catalysis In situ TEM Strong metal-support interaction Structure changes Interfaces Structural evolution

High-efficiency PdNi single-atom alloy catalyst toward cross-coupling reaction

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Chinese Chemical Letters 2024年第7期35卷 480-483页

作者： Baokang Geng Xiang Chu Li Liu Lingling Zhang Shuaishuai Zhang Xiao Wang Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Department of Chemistry Tsinghua UniversityBeijing 100084China

The preparation of Pd-based catalysts with rich electrons and a high atom dispersion rate is of great significance for improving the reactivity of cross-coupling reactions,which is a powerful tool for pharmaceutical and fine chemical ***,we report a PdNi single-atom alloy(SAA)catalyst in which isolated Pd single atoms are anchored onto the surface of Ni nanoparticles(NPs)applied for Suzuki coupling reactions and Heck coupling *** 0.1%PdNi SAA exhibits extraordinary catalytic activity(reaction rate:17,032.25 mmol h^(-1)gPd^(-1))toward the Suzuki cross-coupling reaction between 4-bromoanisole and phenylboronic acid at 80℃for 1 *** excellent activity is supposed to attribute to the 100 percent utilization rate of Pd atoms and the highly stable surface zero-valance Pd atoms,which provides abundant sites and electrons for the adsorption and fracture of the C-X(X=Cl,Br,I)***,our work demonstrates the excellent application prospect of SAAs for cross-coupling reactions.

关键词： Single-atom alloy Cross-coupling reaction Palladium catalysis heterogeneous catalysis High-efficiency