Spurred by the world information tide, China has organized a series of information projects, called the "Three Gold" projects. Recently I had an interview with Mr. Hu Qili, Minister of Electronics Industry, ...Spurred by the world information tide, China has organized a series of information projects, called the "Three Gold" projects. Recently I had an interview with Mr. Hu Qili, Minister of Electronics Industry, about the establishment of China’s modern Electronic Information Industry. Mr. Hu told me that information is the mark of development of a modern society and electronics is the major means of carrying information. Establishing展开更多
Direct conversion of syngas from those non-petroleum carbon resources to higher alcohols are very attractive due to the process simplicity with low energy consumption.However,the reaction always suffers from low yield...Direct conversion of syngas from those non-petroleum carbon resources to higher alcohols are very attractive due to the process simplicity with low energy consumption.However,the reaction always suffers from low yield as well as low selectivity.Herein,effective increase of higher alcohols proportion in the product is realized by direct conversion of syngas over electronically-modulated ZnO semiconductor via Cu doping.It is considered that the lower Fermi level and narrower band gap of catalysts by embedding Cu^(2+)into ZnO lattice could facilitate donor reaction by boosting the process for the reactants to obtain electrons on the catalyst surface for the formation of CH_(x) species and carbon chain growth,in which the Cu doping on ZnO lattice play important role in the promotion of CO adsorption.As a result,4 mol%Cu doped ZnO exhibits a highest C_(2+) OH/ROH fraction of 48.1%.Selectivity of catalysts from straight chain alcohol is better than from branch chain alcohol,which is different from promoted Cu/ZnO based catalyst.However,over-doping of Cu(7 mol%)on ZnO results in the aggregation Cu species on ZnO surface,leading to a sharp decrease of higher alcohols proportion to 3.2%.The results shed light on the nature that a direct correlation between semiconductor Fermi level and synthesis of higher alcohols,and the semiconductor-based catalysts mainly accelerate the hydrogenation reactions by enhancing thermally excited electron transfer.展开更多
Nitrogen chemisorption is a prerequisite for efficient ammonia synthesis under ambient conditions,but promoting this process remains a significant challenge.Here,by loading yttrium clusters onto a single-atom support,...Nitrogen chemisorption is a prerequisite for efficient ammonia synthesis under ambient conditions,but promoting this process remains a significant challenge.Here,by loading yttrium clusters onto a single-atom support,an electronic promoting effect is triggered to successfully eliminate the nitrogen chemisorption barrier and achieve highly efficient ammonia synthesis.Density functional theory calculations reveal that yttrium clusters with abundant electron orbitals can provide considerable electrons and greatly promote electron backdonation to the N2 antibonding orbitals,making the chemisorption process exothermic.Moreover,according to the“hot atom”mechanism,the energy released during exothermic N2 chemisorption would benefit subsequent N2 cleavage and hydrogenation,thereby dramatically reducing the energy barrier of the overall process.As expected,the proof-of-concept catalyst achieves a prominent NH3 yield rate of 48.1μg·h^(−1)·mg^(−1)at−0.2 V versus the reversible hydrogen electrode,with a Faradaic efficiency of up to 69.7%.This strategy overcomes one of the most serious obstacles for electrochemical ammonia synthesis,and provides a promising method for the development of catalysts with high catalytic activity and selectivity.展开更多
文摘Spurred by the world information tide, China has organized a series of information projects, called the "Three Gold" projects. Recently I had an interview with Mr. Hu Qili, Minister of Electronics Industry, about the establishment of China’s modern Electronic Information Industry. Mr. Hu told me that information is the mark of development of a modern society and electronics is the major means of carrying information. Establishing
基金support by the National Natural Science Foundation of China(21975173 and 21776195)the fund for Shanxi“1331 project”and Major Projects of Shanxi Province(201803D121043).
文摘Direct conversion of syngas from those non-petroleum carbon resources to higher alcohols are very attractive due to the process simplicity with low energy consumption.However,the reaction always suffers from low yield as well as low selectivity.Herein,effective increase of higher alcohols proportion in the product is realized by direct conversion of syngas over electronically-modulated ZnO semiconductor via Cu doping.It is considered that the lower Fermi level and narrower band gap of catalysts by embedding Cu^(2+)into ZnO lattice could facilitate donor reaction by boosting the process for the reactants to obtain electrons on the catalyst surface for the formation of CH_(x) species and carbon chain growth,in which the Cu doping on ZnO lattice play important role in the promotion of CO adsorption.As a result,4 mol%Cu doped ZnO exhibits a highest C_(2+) OH/ROH fraction of 48.1%.Selectivity of catalysts from straight chain alcohol is better than from branch chain alcohol,which is different from promoted Cu/ZnO based catalyst.However,over-doping of Cu(7 mol%)on ZnO results in the aggregation Cu species on ZnO surface,leading to a sharp decrease of higher alcohols proportion to 3.2%.The results shed light on the nature that a direct correlation between semiconductor Fermi level and synthesis of higher alcohols,and the semiconductor-based catalysts mainly accelerate the hydrogenation reactions by enhancing thermally excited electron transfer.
基金supported by the National Natural Science Foundation of China(Nos.U21A20332,52103226,and 52071226)the Outstanding Youth Foundation of Jiangsu Province(No.BK20220061)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20201171)the Key Research and Development Plan of Jiangsu Province(No.BE2020003-3)the Fellowship of China Postdoctoral Science Foundation(No.2021M702382).
文摘Nitrogen chemisorption is a prerequisite for efficient ammonia synthesis under ambient conditions,but promoting this process remains a significant challenge.Here,by loading yttrium clusters onto a single-atom support,an electronic promoting effect is triggered to successfully eliminate the nitrogen chemisorption barrier and achieve highly efficient ammonia synthesis.Density functional theory calculations reveal that yttrium clusters with abundant electron orbitals can provide considerable electrons and greatly promote electron backdonation to the N2 antibonding orbitals,making the chemisorption process exothermic.Moreover,according to the“hot atom”mechanism,the energy released during exothermic N2 chemisorption would benefit subsequent N2 cleavage and hydrogenation,thereby dramatically reducing the energy barrier of the overall process.As expected,the proof-of-concept catalyst achieves a prominent NH3 yield rate of 48.1μg·h^(−1)·mg^(−1)at−0.2 V versus the reversible hydrogen electrode,with a Faradaic efficiency of up to 69.7%.This strategy overcomes one of the most serious obstacles for electrochemical ammonia synthesis,and provides a promising method for the development of catalysts with high catalytic activity and selectivity.