Recently, metal clusters supported on some solids which simultaneously exhibit many excellent properties of both metal clusters and supports have been intensively studled. Such surface organometallic chemistry, which ...Recently, metal clusters supported on some solids which simultaneously exhibit many excellent properties of both metal clusters and supports have been intensively studled. Such surface organometallic chemistry, which concerns the synthesis, structure, reactivity and catalytic activity of surface-supported organometallfc compounds is a new展开更多
Although driven by different research interests,single-site catalysts and single-atom catalysts are both believed to be model systems bridging homogeneous and heterogeneous catalysis.The two concepts are similar but d...Although driven by different research interests,single-site catalysts and single-atom catalysts are both believed to be model systems bridging homogeneous and heterogeneous catalysis.The two concepts are similar but different.In this review,we will first explain the difference between single-atom catalysis and single-site catalysis,in terms of their goals,synthetic methods and coordination structures of corresponding catalysts.Then,we will introduce the surface organometallic chemistry method,a method traditionally used for synthesizing single-site catalyst.We will explain why it might benefit the single-atom catalysis community.At last,the choice of support to accommodate the method for synthesizing single-atom catalysts will be discussed.展开更多
The cycloaddition of CO_(2) to epoxides to afford cyclic organic carbonates is an increasingly relevant non-reductive strategy to convert CO_(2) to useful products able to serve as high-boiling solvents,chemical inter...The cycloaddition of CO_(2) to epoxides to afford cyclic organic carbonates is an increasingly relevant non-reductive strategy to convert CO_(2) to useful products able to serve as high-boiling solvents,chemical intermediates,and monomers for the preparation of more sustainable polymers.The development of efficient and robust hetero-geneous catalysts for such transformation is,therefore,crucial and can be carried out by several strategies that often require the preparation of sophisticated and/or expensive organic networks,linkers,or compounds.A different approach to the preparation of heterogeneous catalysts for CO_(2)-epoxide coupling is by applying surface science methodologies to graft molecular fragments or single atoms on various supports leading to well-defined active sites.In this context,surface organometallic chemistry(SOMC),along with comparable methodologies,is a valuable approach for the preparation of efficient,single-site Lewis acids and catalysts for the target cycloaddition reaction on metal oxides,whereas,other grafting methodologies,can be applied to prepare analogous catalysts on different kinds of surfaces.Finally,we discuss very recent advances in the application of surface methodologies for the preparation of single atom catalysts as an increasingly relevant approach towards highly active Lewis acids for the cycloaddition of CO_(2) to epoxides.Overall,we show that Lewis acids and catalysts prepared by facile surface methodologies hold significant potential for future application is the synthesis of cyclic carbonates from CO_(2).展开更多
文摘Recently, metal clusters supported on some solids which simultaneously exhibit many excellent properties of both metal clusters and supports have been intensively studled. Such surface organometallic chemistry, which concerns the synthesis, structure, reactivity and catalytic activity of surface-supported organometallfc compounds is a new
基金ShanghaiTech University Start-up Funding and the Shanghai Pujiang Talent Program,China(No.21PJ1410400).
文摘Although driven by different research interests,single-site catalysts and single-atom catalysts are both believed to be model systems bridging homogeneous and heterogeneous catalysis.The two concepts are similar but different.In this review,we will first explain the difference between single-atom catalysis and single-site catalysis,in terms of their goals,synthetic methods and coordination structures of corresponding catalysts.Then,we will introduce the surface organometallic chemistry method,a method traditionally used for synthesizing single-site catalyst.We will explain why it might benefit the single-atom catalysis community.At last,the choice of support to accommodate the method for synthesizing single-atom catalysts will be discussed.
基金V.D.E.thanks the National Research Council of Thailand(NRCT)(grants Nos.N41A640170 and N42A650196)for funding this work.A.W.K.is grateful to Cerca program/Generalitat de Catalunya,ICREA,Ministerio de Ciencia e Innovacion(PID2020-112684GB-100Severo Ochoa Excellence Accreditation 2020-2023 CEX2019-000925-S).
文摘The cycloaddition of CO_(2) to epoxides to afford cyclic organic carbonates is an increasingly relevant non-reductive strategy to convert CO_(2) to useful products able to serve as high-boiling solvents,chemical intermediates,and monomers for the preparation of more sustainable polymers.The development of efficient and robust hetero-geneous catalysts for such transformation is,therefore,crucial and can be carried out by several strategies that often require the preparation of sophisticated and/or expensive organic networks,linkers,or compounds.A different approach to the preparation of heterogeneous catalysts for CO_(2)-epoxide coupling is by applying surface science methodologies to graft molecular fragments or single atoms on various supports leading to well-defined active sites.In this context,surface organometallic chemistry(SOMC),along with comparable methodologies,is a valuable approach for the preparation of efficient,single-site Lewis acids and catalysts for the target cycloaddition reaction on metal oxides,whereas,other grafting methodologies,can be applied to prepare analogous catalysts on different kinds of surfaces.Finally,we discuss very recent advances in the application of surface methodologies for the preparation of single atom catalysts as an increasingly relevant approach towards highly active Lewis acids for the cycloaddition of CO_(2) to epoxides.Overall,we show that Lewis acids and catalysts prepared by facile surface methodologies hold significant potential for future application is the synthesis of cyclic carbonates from CO_(2).
