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Polymer-supported chiral palladium-based complexes as efficient heterogeneous catalysts for asymmetric reductive Heck reaction

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Green Synthesis and Catalysis

Green Synthesis and catalysis 2024年第2期5卷 102-107页

作者： Hui Zhang Bing Xu Liejin Zhou Zhan-Ming Zhang Junliang Zhang College of Marine Ecology and Environment Shanghai Ocean University999 Hucheng Ring RoadShanghai 201306China Department of Chemistry Fudan University2005 Songhu RoadShanghai 200438China Graduate School of Pharmaceutical Sciences Tohoku UniversitySendai 980-8578Japan Fudan Zhangjiang Institute Shanghai 201203China

heterogeneous asymmetric catalysis is an important strategy for the industrial production of chiral ***,we reported a polymer-bound Xu-Phos-derived palladium catalyst that shows good performance in heterogeneous asymmetric reductive Heck reaction of allyl aryl *** heterogeneous catalyst was easily prepared by efficient immobilization of the sulfonamide phosphine ligand(Xu-Phos)in the cross-linked polystyrene via copolymerization,and exhibits similar catalytic activity and enantioselectivity to that of the homogeneous ***,the heterogeneous catalyst system is proved to be easily recovered and reused several times without losing catalytic activity obviously.

关键词： heterogeneous catalysis Recoverability Palladium Hydroarylation Asymmetric catalysis

Toward Next-Generation heterogeneous Catalysts:Empowering Surface Reactivity Prediction with Machine Learning

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Engineering 2024年第8期39卷 25-44页

作者： Xinyan Liu Hong-Jie Peng Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731China

heterogeneous catalysis remains at the core of various bulk chemical manufacturing and energy conversion processes,and its revolution necessitates the hunt for new materials with ideal catalytic activities and economic *** high-throughput screening presents a viable solution to this challenge,as machine learning(ML)has demonstrated its great potential in accelerating such processes by providing satisfactory estimations of surface reactivity with relatively low-cost *** review focuses on recent progress in applying ML in adsorption energy prediction,which predominantly quantifies the catalytic potential of a solid *** models that leverage inputs from different categories and exhibit various levels of complexity are classified and *** the end of the review,an outlook on the current challenges and future opportunities of ML-assisted catalyst screening is *** believe that this review summarizes major achievements in accelerating catalyst discovery through ML and can inspire researchers to further devise novel strategies to accelerate materials design and,ultimately,reshape the chemical industry and energy landscape.

关键词： Machine learning heterogeneous catalysis Chemisorption Theoretical simulation Materials design High-throughput screening

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通过二维沸石调节铂的氢化选择性

Science China Materials 2024年第7期67卷 2135-2141页

作者：翟玉慧马悦崔凤超田宇阳朱广山 Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

不饱和醇是一类重要的医药中间体,然而C=C加氢比C=O加氢反应更具有热力学优势,因此由不饱和醛合成不饱和醇具有挑战性.为解决这一问题,需要寻求一种具有可调控选择性的氢化催化剂.二维沸石的高长径比和大量的末端基团作为锚定位点,使其... 详细信息

不饱和醇是一类重要的医药中间体,然而C=C加氢比C=O加氢反应更具有热力学优势,因此由不饱和醛合成不饱和醇具有挑战性.为解决这一问题,需要寻求一种具有可调控选择性的氢化催化剂.二维沸石的高长径比和大量的末端基团作为锚定位点,使其不仅能作为催化剂载体,还可以有效地调节催化剂性能.本研究利用二维沸石IPC-1P作为铂纳米颗粒的载体,成功制备出异相催化剂Pt@IPC-1P.铂纳米颗粒的尺寸小于2 nm且均匀地分布在IPC-1P上.令人惊喜的是,Pt@IPC-1P催化剂对不饱和醇的选择性超过了90%,并实现了接近100%的催化转化率,远超其他铂基催化剂.理论计算证实,二维沸石IPC-1P在肉桂醛向肉桂醇的转化过程中起到了积极作用,其放热效应能量高于苯丙醛.这项工作展现了二维沸石在催化有机物转化领域具有广阔的应用前景.

关键词： heterogeneous catalysis 2D zeolite hydrogenation selectivity cinnamaldehyde top-down approach

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Unveiling the relationship between structural evaluation and catalytic performance of InOOH during electroreduction of CO_(2)to formate

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Green Carbon 2024年第1期2卷 124-130页

作者： Caijun Deng Chaofan Qi Xiaomin Wu Guohua Jing Huawang Zhao Department of Environmental Science&Engineering College of Chemical EngineeringHuaqiao UniversityXiamenFujian 361021 China

The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into ***,the indeterminate mechanism underlying structural self-reconstruction obstructs the strategic design of a high-performance In catalyst for the ECO_(2)*** this study,we chose InOOH as the model catalyst to illustrate the dynamic structure of In-based catalysts during reconstruction in the ECO_(2)*** findings of the current study indicate that the in situ electrochemical reconstruction of crystalline InOOH results in the creation of crystalline In clusters/InOOH,followed by In/InOOH heterostructures,and finally,metallic In over *** efficiencies of the different phases conformed to the sequence:In clusters/InOOH>In/InOOH heterostructures>metallic *** progression leads to a continuous drop in maximum current density and Faradaic efficiency from 29.6 mA/cm2 and 87%to 6.3 mA/cm^(2) and 75%,respectively with time extending to 7200 s,at-1.0 V relative to the reversible hydrogen *** in situ characterization and theoretical studies highlighted the crucial role of the In-cluster/InOOH interface in CO_(2)activation and conversion.

关键词： Indium Carbon dioxide reduction electrochemistry Formic acid heterogeneous catalysis

Selective sulfur conversion with surface engineering of electrocatalysts in a lithium-sulfur battery

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Carbon Energy 2023年第2期5卷 72-84页

作者： Yuejin Zhu Yinze Zuo Xuechao Jiao Revanasiddappa Manjunatha Ejikeme Raphael Ezeigwe Wei Yan Jiujun Zhang Institute for Sustainable Energy College of SciencesShanghai UniversityShanghaiPR China College of Materials Science and Engineering Fuzhou UniversityFuzhouPR China

The sluggish kinetics of multiphase sulfur conversion with homogeneous and heterogeneous electrochemical processes,causing the“shuttle effect”of soluble polysulfide species(PSs),is the challenges in terms of lithium-sulfur batteries(LSBs).In this paper,a Mn_(3)O_(4-x) catalyst,which has much higher activity for heterogeneous reactions than for homogeneous reactions(namely,preferentialactivity catalysts),is designed by surface engineering with rational oxygen *** to the rational design of the electronic structure,the Mn_(3)O_(4-x) catalyst prefers to accelerate the conversion of Li2S4 into Li_(2)S_(2)/Li_(2)S and optimize Li_(2)S deposition,reducing the accumulation of PSs and thus suppressing the“shuttle effect.”Both density functional theory calculations and in situ X-ray diffraction measurements are used to probe the catalytic mechanism and identify the reaction intermediates of MnS and Li_(y)Mn_(z)O_(4-x) for fundamental *** cell with Mn_(3)O_(4-x) delivers an ultralow attenuation rate of 0.028% per cycle over 2000 cycles at 2.5 *** with sulfur loadings of 4.93 and 7.10mg cm^(-2) in a lean electrolyte(8.4μL mg s^(-1)),the cell still shows an initial areal capacity of 7.3mAh cm^(-2).This study may provide a new way to develop preferential-activity heterogeneous-reaction catalysts to suppress the“shuttle effect”of the soluble PSs generated during the redox process of LSBs.

关键词： electrochemical kinetics heterogeneous catalysis lithium-sulfur batteries Mn3O4-x-catalyzed separator surface engineering

Breaking the activity limitation of iridium single-atom catalyst in hydrogenation of quinoline with synergistic nanoparticles catalysis

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Nano Research 2022年第6期15卷 5024-5031页

作者： Qikai Shen Hongqiang Jin Peipei Li Xiaohu Yu Lirong Zheng Weiguo Song Changyan Cao Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesCAS Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Institute of Theoretical and Computational Chemistry Shaanxi Key Laboratory of CatalysisSchool of Chemical&Environment SciencesShaanxi University of TechnologyHanzhong 723000China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China

Single-atom catalysts(SACs)with the advantages of homogeneous and heterogeneous catalysts have become a hot-spot in catalysis ***,for lack of metal–metal bond in SACs,H_(2)has to go through heterolytic dissociation pathway,which has higher barrier than homolytic dissociation pathway,and thus limits the hydrogenation activity of ***,we propose and demonstrate through constructing synergistic iridium single atoms and nanoparticles co-existed catalyst(denoted as Ir_(1+NPs)/CMK)to boost the catalytic activity of quinoline *** experimental and density functional theory calculation results confirm that Ir_(1)single sites activate quinoline,while Ir nanoparticles boost hydrogen dissociation.H atoms generated at Ir nanoparticles migrate to the quinoline bounded Ir_(1)single sites to complete *** Ir_(1+NPs)/CMK catalyst exhibits much higher reactivity with turnover frequency of 7,800 h^(−1)than those counterpart Ir_(1)/CMK and IrNPs/CMK catalysts,and is 20,000 times higher activity of commercial Ir/C benchmark catalyst for hydrogenation of quinoline under the same reaction *** synergistic catalysis strategy between single atoms and nanoparticles provides a solution to further improve the performance of SACs for hydrogenation.

关键词： heterogeneous catalysis single atom synergistic quinoline hydrogenation

Solid-solution alloy nanoclusters of the immiscible gold-rhodium system achieved by a solid ligand-assisted approach for highly efficient catalysis

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Nano Research 2020年第1期13卷 105-111页

作者： Xinchun Yang Zhangpeng Li Mitsunori Kitta Nobuko Tsumori Wenhan Guo Zitao Zhang Jianbo Zhang Ruqiang Zou Qiang Xu Institute of Electrochemical Energy National Institute of Advanced Industrial Science and Technology(AIST)IkedaOsaka563-8577Japan Graduate School of Engineering Kobe UniversityNada KuKobeHyogo657-8501Japan Department of Applied Chemistry and Chemical Engineering Toyama National College of TechnologyToyama939-8630Japan Department of Materials Science and Engineering Peking UniversityBeijing100871China Centre for High-Pressure Science and Technology Advanced Research Beijing100094China AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory YoshidaSakyo-kuKyoto606-8501Japan

Striking effects are expected in solid-solution alloying,which offers enormous possibilities for various applications,especially in industrial ***,phase diagrams have revealed that a wide range of metallic elements are immiscible with each other even above their melting *** such unknown alloying between different immiscible metallic elements is highly desirable but ***,for the first time,by using an innovative solid ligand-assisted approach,we achieve the solid-solution alloying between the bulk-immiscible Au and Rh in plenty of clean,ultrafine(∼1.6 nm)and highly dispersed *** solid-solution alloying of immiscible Au and Rh significantly enhances their catalytic performance toward the hydrogen evolution from formic acid in contrast to the monometallic Au and Rh ***,the resultant binary solid-solution nanoclusters are stable without any segregation during catalytic *** approach demonstrated here for homogeneously mixing the immiscible metals at the atomic scale will benefit the creation of advanced alloys and their catalytic applications in future.

关键词： solid-solution alloys metal nanoclusters formic acid dehydrogenation heterogeneous catalysis

Single-atom catalyst: a rising star for green synthesis of fine chemicals

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National Science Review 2018年第5期5卷 653-672页

作者： Leilei Zhang Yujing Ren Wengang Liu Aiqin Wang Tao Zhang State Key Laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences

The green synthesis of fine chemicals calls for a new generation of efficient and robust catalysts. Single-atom catalysts(SACs), in which all metal species are atomically dispersed on a solid support, and which often consist of well-defined mononuclear active sites, are expected to bridge homogeneous and heterogeneous catalysts for liquid-phase organic transformations. This review summarizes major advances in the SAC-catalysed green synthesis of fine chemicals in the past several years, with a focus on the catalytic activity, selectivity and reusability of SACs in various organic reactions. The relationship between catalytic performance and the active site structure is discussed in terms of the valence state, coordination environment and anchoring chemistry of single atoms to the support, in an effort to guide the rational design of SACs in this special area, which has traditionally been dominated by homogeneous ***, the challenges remaining in this research area are discussed and possible future research directions are proposed.

关键词： single-atom catalysts fine chemicals green synthesis structure–reactivity relationship heterogeneous catalysis

For more and purer hydrogen-the progress and challenges in water gas shift reaction

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能源化学:英文版 2023年第8期83卷 363-396,I0010页

作者： Limin Zhou Yanyan Liu Shuling Liu Huanhuan Zhang Xianli Wu Ruofan Shen Tao Liu Jie Gao Kang Sun Baojun Li Jianchun Jiang 218 Laboratory for Energy catalysis Research Center of Green CatalysisCollege of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina Institute of Chemical Industry of Forest Products CAFNational Engineering Lab.for Biomass Chemical UtilizationNanjing 210042JiangsuChina College of Science Henan Agricultural UniversityZhengzhou 450002HenanChina National Center for Nanoscience and Technology Beijing 100190China School of Life Sciences Northwestern Polytech UniversityXi'an 710072ShaanxiChina

The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to ammonia synthesis and other reactions. Advanced catalysts have been developed for both high and low-temperature reactions and are widely used in industry. In recent years, supported metal nanoparticle catalysts have been researched due to their high metal utilization. Low-temperature catalysts have shown promising results, including high selectivity, high shift rates, and higher activity potential. Additionally, significant progress has been made in removing trace CO through the redox reaction in electrolytic cell. This paper reviews the development of WGS reaction catalysts, including the reaction mechanism, catalyst design, and innovative research methods. The catalyst plays a crucial role in the WGS reaction, and this paper provides an instant of catalyst design under different conditions. The progress of catalysts is closely related to the development of advanced characterization ***, modifying the catalyst surface to enhance activity and significantly increase reaction kinetics is a current research direction. This review goals to stimulate a better understanding of catalyst design, performance optimization, and driving mechanisms, leading to further progress in this field.

关键词： Water gas shift reaction Hydrogen production heterogeneous catalysis Reaction Mechanism Single atomic catalysts

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