Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, ...Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, however, high temperature, high pressure, and high-purity CO_(2) are still required for the reaction.Here, we report two new Zn(Ⅱ) imidazolate frameworks incoporating MoO_(4)^(2–)or WO_(4)^(2–)units, which can catalyse cycloaddition of CO_(2) and epichlorohydrin at room temperature and atomospheric pressure, giving 95% yield after 24 h in pure CO_(2) and 98% yield after 48 h in simulated flue gas(15% CO_(2)+ 85% N_(2)),respectively. For comparison, the analogic Zn(Ⅱ) imidazolate framework MAF-6 without non-3d metal oxide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO_(4)^(2–)unit in optimizing the electronic structure of Zn(Ⅱ) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations.展开更多
As electronic packages become more compact, run at faster speeds and dissipate more heat, package designers need more effective thermal management materials. CVD diamond, because of its high thermal conductivity, low ...As electronic packages become more compact, run at faster speeds and dissipate more heat, package designers need more effective thermal management materials. CVD diamond, because of its high thermal conductivity, low dielectric loss and its great mechanical strength, is an excellent material for three dimensional (319) multichip modules (MCMs) in the next generation compact high speed computers and high power microwave components. In this paper, we have synthesized a large area freestanding diamond films and substrates, and polished diamond substrates, which make MCMs diamond film sink becomes a reality.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 22090061, 21731007, 21890380 and 22161021)the Guangdong Pearl River Talents Program (No. 2017BT01C161)the support of Jiangxi Province (No. jxsq2018106041)。
文摘Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, however, high temperature, high pressure, and high-purity CO_(2) are still required for the reaction.Here, we report two new Zn(Ⅱ) imidazolate frameworks incoporating MoO_(4)^(2–)or WO_(4)^(2–)units, which can catalyse cycloaddition of CO_(2) and epichlorohydrin at room temperature and atomospheric pressure, giving 95% yield after 24 h in pure CO_(2) and 98% yield after 48 h in simulated flue gas(15% CO_(2)+ 85% N_(2)),respectively. For comparison, the analogic Zn(Ⅱ) imidazolate framework MAF-6 without non-3d metal oxide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO_(4)^(2–)unit in optimizing the electronic structure of Zn(Ⅱ) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations.
基金Supported by National Natural Science Foundation of China (No.60371006)
文摘As electronic packages become more compact, run at faster speeds and dissipate more heat, package designers need more effective thermal management materials. CVD diamond, because of its high thermal conductivity, low dielectric loss and its great mechanical strength, is an excellent material for three dimensional (319) multichip modules (MCMs) in the next generation compact high speed computers and high power microwave components. In this paper, we have synthesized a large area freestanding diamond films and substrates, and polished diamond substrates, which make MCMs diamond film sink becomes a reality.