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single-atom catalysis for organic reactions

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Chinese Chemical Letters 2023年第6期34卷 121-129页

作者： Hanyu Hu Jiangbo Xi Key Laboratory of Novel Biomass-Based Environmental and Energy Materials in Petroleum and Chemical Industry Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemistry and Environmental EngineeringWuhan Institute of TechnologyWuhan 430205China

Metal-based catalysis,including homogeneous and heterogeneous catalysis,plays a significant role in the modern chemical *** catalysis is widely used due to the high efficiency,easy catalyst separation and ***,the metal-utilization efficiency for conventional heterogeneous catalysts needs further improvement compared to homogeneous *** tackle this,the pursing of heterogenizing homogeneous catalysts has always been attractive but *** a recently emerging class of catalytic material,single-atom catalysts(SACs)are expected to bridge homogeneous and heterogeneous catalytic process in organic reactions and have arguably become the most active new frontier in catalysis *** this review,a brief introduction and development history of single-atom catalysis and SACs involved organic reactions are *** addition,recent advances in SACs and their practical applications in organic reactions such as oxidation,reduction,addition,coupling reaction,and other organic reactions are thoroughly *** understand structure-property relationships of single-atom catalysis in organic reactions,active sites or coordination structure,metal atom-utilization efficiency(e.g.,turnover frequency,TOF calculated based on active metal)and catalytic performance(e.g.,conversion and selectivity)of SACs are comprehensively ***,the application limitations,development trends,future challenges and perspective of SAC for organic reaction are discussed.

关键词： single-atom catalysis Active site Metal utilization Organic reaction Catalytic performance

Ensemble of single-atom catalysis and defect engineering in Cu_(1)/CeO_(2) nanozymes for tumor therapy

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中国科学:化学英文版 2023年第9期66卷 2590-2599页

作者： Hao-Xin Liu Zhiliang Gao Han Yan Shan-Qing Li Wei-Wei Wang Xuetao Qin Hongning Sun Jiwei Cui Chun-Jiang Jia Key Laboratory of Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials of the Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China School of Materials and Environmental Engineering Chizhou UniversityChizhou 247000China

As a class of nanomaterials with natural enzyme-like characteristics, nanozymes have shown their great potential in various applications. Reducible metal oxides featured with defect structures, and single-atom catalysts with isolated metal sites are regarded as two of the most promising nanozymes. However, the strategies to construct highly performed nanozymes by combining these advantages are rarely reported. Herein, we report the coordination-unsaturated single-atomic Cu species supported on sintered CeO_(2), which combines the advantages of defect engineering and single-atom catalysis, exhibiting a largely enhanced peroxidase(POD)-like activity. The high-temperature calcination induces the transformation of inert Cu_(1)O_(4) species into coordination-unsaturated Cu_(1)O_(3) sites. This novel Cu_(1)O_(3) active sites with an unsaturated coordination work as a new type of defect sites to greatly activate the isolated Cu atoms and accelerate the dissociation of H_(2)O_(2) to form hydroxyl radicals(·OH). The obtained nanozyme with a high POD-like activity possesses low cytotoxicity, showing potential applications for the tumor inhibition in vitro and in vivo.

关键词： single-atom catalysis oxygen defect Cu/CeO_(2) peroxidase-like activity tumor inhibition

single-atom catalysis: Bridging the homo-and heterogeneous catalysis

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Chinese Journal of catalysis 2018年第5期39卷 893-898页

作者： Fang Chen Xunzhu Jiang Leilei Zhang Rui Lang Botao Qiao State Key Laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina School of Chemistry Dalian University of TechnologyDalian 116024LiaoningChina

single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis *** have the advantages of both homogeneous catalysts(isolated active sites)and heterogeneous catalysts(stable and easy to separate),and are thus predicted to be able to bridge the homo-and heterogeneous *** prediction was first experimentally demonstrated in *** this mini-review,we summarize the few homogeneous catalysis progresses reported recently where SACs have exhibited promising application:a)Rh/ZnO and Rh/CoO SAC have been used successfully in hydroformylation of olefin of which the activity are comparable to the homogeneous Wilkinson’s catalyst;b)a Pt/Al2O3 SAC has shown excellent performance in hydrosilylation reaction;and c)M-N-C SACs(M=Fe,Co etc.)have been applied in the activation of C–H *** of these examples suggest that fabrication of suitable SACs could provide a new avenue for the heterogenization of homogeneous *** pioneering works shed new light on the recognition of single-atom catalysis in bridging the homo-and heterogeneous catalysis.

关键词： single-atom catalysis Heterogenization of homogeneous catalysts Hydroformation Hydrosilylation Activation of C–H bonds

single-atom catalysis enables long-life, high-energy lithium-sulfur batteries

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Nano Research 2020年第7期13卷 1856-1866页

作者： Zechao Zhuang Qi Kang Dingsheng Wang Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China

With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past *** applications of LSBs ranging from electric vehicles to stationary grid storage seem rather bright in recent ***,there still exist many pressing challenges to be addressed because we do not yet fully understand and control the electrode-electrolyte interface chemistries during battery operation,such as polysulide shuttling and poor utilization of active ***-atom catalysts(SACs)pave new possibilities of tackling the tough issues due to their decent applicability in the atomic-level identification of structure-activity relationships and reaction mechanism,as well as their structural tunability with atomic *** review comprehensively summarizes the very recent advances in utilization of highly active SACs for LSBs by stating and discussing the related publications,which involves catalyst synthesis routes,battery pertormance,catalytic mechanisms,optimization strategies,and promises to achieve long-lite,high-energy *** see that endeavors to employ SACs to modify sulfur cathode have allowed efficient polysulfide conversion and confinement,leading to the minimization of shuttle *** efforts are being devoted to extending the scope of SACs to cell separator and lithium metal anode in order to unlock the full potential of *** also obtain mechanistic insights into battery chemistries and nature of SACs in their strong interactions with polysulfides through advanced in situ characterizations ***,acceleration in the development of LSBs by introducing SACs is noticeable,and this cutting edge needs more attentions to further promoting the design of better LSBs.

关键词： single-atom catalysis lithium-sulfur battery polysulfide conversion shuttle effect atomic-level insight

single-atom catalysis: a new field that learns from tradition

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National Science Review 2018年第5期5卷 690-693页

作者： Philip Ball NSR

Much of industrial chemical processing (in the petrochemicals industry, for example), and a great deal of laboratory chemical synthesis,involves catalysts that both lower the energy barrier to reaction and may help steer a reaction along a particular path. Traditionally,catalysts have come in two classes:heterogeneous, typically meaning that the catalyst is an extended solid; and homogeneous, where the catalyst is a small molecule that shares a solvent with the reactants. In heterogeneous catalysis, the reaction generally takes place on a

关键词： single-atom catalysis

D-band center coordination modulated enzyme-like activity in Fe-Cu dual-metal single-atom nanozymes

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Nano Research 2024年第7期17卷 5872-5883页

作者： Ling Liu Shaofang Zhang Guo Li Yadong Zhe Jiamin Liu Xinxu Zhang Jiahao Wei Xin Sun Yonghui Li Xiao-Dong Zhang Tianjin Key Laboratory of Brain Science and Neural Engineering Academy of Medical Engineering and Translational MedicineTianjin UniversityTianjin 300072China Department of Physics and Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology School of SciencesTianjin UniversityTianjin 300350China

After explorations in a diversity of single-atom nanozymes(SAzymes),developing dual-centered SAzymes becomes a promising approach for superior catalytic *** confusing mechanisms including atomic coordination,spatial configuration,and metal–metal atom interaction hinder the development and design of ***,a dual-centered Fe-Cu-N_(x)SAzyme exhibits excellent peroxidase(POD)-and catalase(CAT)-like activities with d-band center(ε_(d))coordination of Fe and Cu in multiple reaction stages,which plays a critical role in the adsorption of H_(2)O_(2)molecule and H_(2)O and O_(2)***,the dband center coordination,which can be represented byε_(d)(Fe)–ε_(d)(Cu)shifts,leads to the competition between one-side and bilateral adsorption,which determines the favorable reaction path with lower energy *** on experimental statistics,simulated formation energies,and reaction barriers,3 configurations,Fe-Cu-N6-I,Fe-Cu-N_(8)-II,and Fe-Cu-N_(8)-III,are modeled and ***,configuration-dependent catalytic selectivity and the competition between one-side and bilateral adsorption can be unveiled by d-band center coordination paradigm *** simulations suggest that the unsymmetrical charge distribution over the three Fe-Cu configurations could tune the adsorption strength compared with the counterparts FeN_(4)and CuN_(4).The present work provides a potential route for optimizing enzyme-like catalysis by designing the dual-or even triple-metal SAzymes,which demonstrates the large space to modulate the metal atomic configuration and interaction.

关键词： single-atom catalysis Fe-Cu dual-metal d-band center coordination enzyme mimicking competitive adsorption mechanisms

Direct synthesis of a disinfectant with fresh scent of green plants by semi-hydrogenation of alkynol on Pd single-atom catalysts

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Nano Research 2024年第5期17卷 3872-3878页

作者： Yan Jiang Xuetong Yu Yuxia Ji Xunzhu Jiang Yalin Guo Tianbo Li Liang Gao Rui Lang Yanxiong Fang Botao Qiao Jinxiang Dong School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China CAS Key Laboratory of Science and Technology on Applied catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116024China Guangdong Provincial Key Laboratory of Plant Resources Biorefinery Guangzhou 510006China School of Chemical Engineering and Technology China University of Mining and TechnologyXuzhou 221116China

Alcohol-based disinfectants have protected people in the coronavirus disease 2019(COVID-19)pandemic,but olfactory stimuli of ethanol may evoke unpleasant memories associated with stressful situations in the devastating infectious *** smell of ethanol in household cleaning and disinfectant products can be covered up by the fragrance additives,and 3-hexenol is especially appreciated for the characteristic,strong odor of green *** production of 3-hexenol relies on the selective hydrogenation of 3-hexyn-1-ol,where Lindlar catalyst is normally used for the superior *** achieving such catalytic transformation in ethanol solution seems as a direct way to produce a disinfectant with green aroma,a popular consumer product in the post-COVID era,severe leaching of toxic Pb hinders Lindlar catalyst as a promising *** find that the Fe_(2)O_(3) supported Pd single-atom catalyst is highly selective to fulfill semi-hydrogenation of 3-hexyn-1-ol in 75%ethanol,and the aforementioned household product is readily generated after filtrating the stable,solid catalyst out of reaction ***-atom catalysts have been frequently utilized for fine-chemical synthesis,while in this work they make stunning debut in practical manufacture of daily used products.

关键词： single-atom catalysis hydrogenation fragrance household product coronavirus disease 2019(COVID-19)

single-atom nanozymes towards central nervous system diseases

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Nano Research 2023年第4期16卷 5121-5139页

作者： Weichen Wei Department of Nanoengineering University of California San DiegoLa Jolla 92093USA

Nanozymes have a similar catalytic mechanism to natural enzymes,with excellent performance,facile synthesis,and better ***-atom nanozymes are developed based on single-atom catalysts due to their advantages in coordination structure and electronic configuration,making them highly enzymatic-like biomimetic *** nervous system(CNS)diseases have become one of the biggest killers of human health because they are difficult to diagnose and treat,expensive,and result in serious ***-atom nanozymes have been widely used for biomedical applications,especially in oxidative-stressinduced diseases and most CNS diseases which are closely related to oxidative ***,single-atom nanozymes show promising application prospects for the treatment of CNS *** addition,due to the outstanding material properties and sensitivity of single-atom nanozymes,they also exhibit great advantages in detecting various CNS disease markers for diagnosis.

关键词： single-atom nanozymes single-atom catalysis central nervous system diseases enzyme-like catalysts reactive oxygen species

atomically dispersed N-coordinated Fe-Fe dual-sites with enhanced enzyme-like activities

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Nano Research 2022年第2期15卷 959-964页

作者： Lei Jiao Wei Ye Yikun Kang Yu Zhang Weiqing Xu Yu Wu Wenling Gu Weiyu Song Yujie Xiong Chengzhou Zhu Key Laboratory of Pesticide and Chemical Biology of Ministry of Education International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China College of Material Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China Hefei National Laboratory for Physical Sciences at the Microscale Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

Replacement of enzymes with nanomaterials such as atomically dispersed metal catalysts is one of the most crucial steps in addressing the challenges in *** the breakthroughs of single-atom catalysts in enzyme-mimicking,a fundamental investigation on the development of an instructional strategy is still required for mimicking biatomic/multiatomic active sites in natural enzymes and constructing synergistically enhanced metal atom active ***,Fe_(2)NC catalysts with atomically dispersed Fe-Fe dual-sites supported by the metal-organic frameworks-derived nitrogen-doped carbon are employed as biomimetic catalysts to perform proof-of-concept *** effect of Fe atom number toward typical oxidase(cytochrome C oxidase,NADH oxidase,and ascorbic acid oxidase)and peroxidase(NADH peroxidase and ascorbic acid peroxidase)activities is systematically evaluated by experimental and theoretical investigations.A peroxo-like O_(2) adsorption in Fe_(2)NC nanozymes could accelerate the O-O activation and thus achieve the enhanced enzyme-like *** work achieves the vivid simulation of the enzyme active sites and provides the theoretical basis for the design of high-performance *** a concept application,a colorimetric biosensor for the detection of S^(2-) in tap water is established based on the inhibition of enzyme-like activity of Fe_(2)NC nanozymes.

关键词： nanozymes atomically dispersed dual-metal sites oxidase-like activities single-atom catalysis sensors