The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO2. So far, homogeneous metal complexes have been mainly a...The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO2. So far, homogeneous metal complexes have been mainly applied for such transformations. Here, we describe the synthesis of novel heterogeneous Zn-based catalysts, which were conveniently prepared by pyrolysis of an active- carbon-supported phenanthroline-ligated Zn(OAc)2 complex. Detail structural characterizations proved the existence of single zinc sites in the active material. Compared to a Zn-based nanoparticle (Zn-NP) catalyst, the resulting single metal atom catalyst (SAC) displayed improved activity and stability for the cycloaddition of epoxides. By applying the optimal catalyst, a variety of carbonates were successfully obtained in high yields with good functional group tolerance.展开更多
The production of bulk organic chemicals has a strong impact on our daily life.In this review,an overview of important industrial processes using homogeneous catalysts is given.Using specific carbonylation and hydroge...The production of bulk organic chemicals has a strong impact on our daily life.In this review,an overview of important industrial processes using homogeneous catalysts is given.Using specific carbonylation and hydrogenation case studies,we want to show how basic research can contribute to the development of such processes and what challenges exist in this area of academic research.展开更多
The worldwide energy system developed in the past century is highly dependent on non-renewable fossil feedstocks.Hence,the concentration of carbon dioxide(CO_(2))in the atmosphere has continuously increased from 280 p...The worldwide energy system developed in the past century is highly dependent on non-renewable fossil feedstocks.Hence,the concentration of carbon dioxide(CO_(2))in the atmosphere has continuously increased from 280 ppm(parts per million)to>420 ppm since the industrial revolution[1–5].This excessive emission of CO_(2) causes global warming and ocean acidification.In this context,the Paris Agreement on Climate Change adopted in 2015 recognized the necessity of holding the increase of global average temperature below 2℃,preferably 1.5℃,above pre-industrial levels,and reaching a CO_(2)-neutral process by 2050.展开更多
基金supported by the National Key R&D Program of China(2017YFA0403103)the state of Mecklenburg-Vorpommern and the Bundesministerium für Bildung und Forschung~~
文摘The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO2. So far, homogeneous metal complexes have been mainly applied for such transformations. Here, we describe the synthesis of novel heterogeneous Zn-based catalysts, which were conveniently prepared by pyrolysis of an active- carbon-supported phenanthroline-ligated Zn(OAc)2 complex. Detail structural characterizations proved the existence of single zinc sites in the active material. Compared to a Zn-based nanoparticle (Zn-NP) catalyst, the resulting single metal atom catalyst (SAC) displayed improved activity and stability for the cycloaddition of epoxides. By applying the optimal catalyst, a variety of carbonates were successfully obtained in high yields with good functional group tolerance.
基金the support of the European Research Council(ERC NoNaCat grant no.670986)the Federal Ministry of Education and Research(BMBF)the State of Mecklenburg-Vorpommern.
文摘The production of bulk organic chemicals has a strong impact on our daily life.In this review,an overview of important industrial processes using homogeneous catalysts is given.Using specific carbonylation and hydrogenation case studies,we want to show how basic research can contribute to the development of such processes and what challenges exist in this area of academic research.
基金support from the Alexander von Humboldt Foundation.
文摘The worldwide energy system developed in the past century is highly dependent on non-renewable fossil feedstocks.Hence,the concentration of carbon dioxide(CO_(2))in the atmosphere has continuously increased from 280 ppm(parts per million)to>420 ppm since the industrial revolution[1–5].This excessive emission of CO_(2) causes global warming and ocean acidification.In this context,the Paris Agreement on Climate Change adopted in 2015 recognized the necessity of holding the increase of global average temperature below 2℃,preferably 1.5℃,above pre-industrial levels,and reaching a CO_(2)-neutral process by 2050.