High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,...High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,a widely-utilized“building block”in today’s chemical industry.Thus,it offers an intriguing and promising means to radically change the way of chemical manufacturing and achieve carbon neutrality using renewable energy sources,CO_(2),and water.Albeit with the great potential of HT-CO_(2)RR,this carbon utilization approach,unfortunately,has been suffering coke formation that is seriously detrimental to its energy efficiency and operating lifetime.In recent years,much effort has been added to understanding the mechanism of coke formation,managing reaction conditions to mitigate coke formation,and devising coke-formation-free electrode materials.These investigations have substantially advanced the HT-CO_(2)RR toward a practical industrial technology,but the resulting coke formation prevention strategies compromise activity and energy efficiency.Future research may target exploiting the control over both catalyst design and system design to gain selectivity,energy efficiency,and stability synchronously.Therefore,this perspective overviews the progress of research on coke formation in HT-CO_(2)RR,and elaborates on possible future directions that may accelerate its practical implementation at a large scale.展开更多
In situ capping is an attractive and cost-effective method for remediation of contaminated sediments,but few studies on enhancing contaminant degradation in sediment caps have been reported,especially for chlorinated ...In situ capping is an attractive and cost-effective method for remediation of contaminated sediments,but few studies on enhancing contaminant degradation in sediment caps have been reported,especially for chlorinated benzenes.Electrically enhanced bioactive barrier is a new process for in situ remediation for reducible compounds in soil or sediments.The primary objective of this study is to determine if electrodes in sediment could create a redox gradient and provide electron acceptor/donor to stimulate degradation of chlorinated contaminant.The results demonstrate that graphite electrodes lead to sustainable evolution of hydrogen,displaying zero-order kinetics in the initial stages with different voltages.The constant rates of hydrogen evolution at 3,4,and 5 V are1.05,2.54,and 4.3 nmol·L 1·d 1,respectively.Even higher voltage can produce more hydrogen,but it could not keep long time because the over potentials on electrode surfaces prevent its function.The study shows that 4 V is more appropriate for hydrogen evolution.The measured and evaluated concentration of 1,2,3,5-tetrachlorobenzene in pore water of sediment and concentration of sulfate show that dechlorination is inhibited at higher concentration of sulfate.展开更多
Integration of molybdenum disulfide （MoS2） onto high surface area photocathod is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction （HER）. Semiconductor nanowires （NWs...Integration of molybdenum disulfide （MoS2） onto high surface area photocathod is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction （HER）. Semiconductor nanowires （NWs） are beneficial use in photoelectrochemistry because of their large electrochemically availab surface area and inherent ability to decouple light absorption and the transpo of minority carriers. Here, silicon （Si） NW arrays were employed as a mod photocathode system for MoS2 wrapping, and their solar-driven HER activil was evaluated. The photocathode is made up of a well-defined MoSJTiO2/Si coaxial NW heterostructure, which yielded photocurrent density up to 15 mA/cm2 （at 0 V vs. the reversible hydrogen electrode （RHE）） with goo stability under the operating conditions employed. This work reveals the earth-abundant electrocatalysts coupled with high surface area NW electrod~ can provide performance comparable to noble metal catalysts for photocathod hydrogen evolution.展开更多
文摘High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,a widely-utilized“building block”in today’s chemical industry.Thus,it offers an intriguing and promising means to radically change the way of chemical manufacturing and achieve carbon neutrality using renewable energy sources,CO_(2),and water.Albeit with the great potential of HT-CO_(2)RR,this carbon utilization approach,unfortunately,has been suffering coke formation that is seriously detrimental to its energy efficiency and operating lifetime.In recent years,much effort has been added to understanding the mechanism of coke formation,managing reaction conditions to mitigate coke formation,and devising coke-formation-free electrode materials.These investigations have substantially advanced the HT-CO_(2)RR toward a practical industrial technology,but the resulting coke formation prevention strategies compromise activity and energy efficiency.Future research may target exploiting the control over both catalyst design and system design to gain selectivity,energy efficiency,and stability synchronously.Therefore,this perspective overviews the progress of research on coke formation in HT-CO_(2)RR,and elaborates on possible future directions that may accelerate its practical implementation at a large scale.
基金Supported by the National Natural Science Foundation of China（51108317） the Municipal Natural Science Foundation of Tianjin（12JCQNJC05400）
文摘In situ capping is an attractive and cost-effective method for remediation of contaminated sediments,but few studies on enhancing contaminant degradation in sediment caps have been reported,especially for chlorinated benzenes.Electrically enhanced bioactive barrier is a new process for in situ remediation for reducible compounds in soil or sediments.The primary objective of this study is to determine if electrodes in sediment could create a redox gradient and provide electron acceptor/donor to stimulate degradation of chlorinated contaminant.The results demonstrate that graphite electrodes lead to sustainable evolution of hydrogen,displaying zero-order kinetics in the initial stages with different voltages.The constant rates of hydrogen evolution at 3,4,and 5 V are1.05,2.54,and 4.3 nmol·L 1·d 1,respectively.Even higher voltage can produce more hydrogen,but it could not keep long time because the over potentials on electrode surfaces prevent its function.The study shows that 4 V is more appropriate for hydrogen evolution.The measured and evaluated concentration of 1,2,3,5-tetrachlorobenzene in pore water of sediment and concentration of sulfate show that dechlorination is inhibited at higher concentration of sulfate.
文摘Integration of molybdenum disulfide （MoS2） onto high surface area photocathod is highly desired to minimize the overpotential for the solar-powered hydrogen evolution reaction （HER）. Semiconductor nanowires （NWs） are beneficial use in photoelectrochemistry because of their large electrochemically availab surface area and inherent ability to decouple light absorption and the transpo of minority carriers. Here, silicon （Si） NW arrays were employed as a mod photocathode system for MoS2 wrapping, and their solar-driven HER activil was evaluated. The photocathode is made up of a well-defined MoSJTiO2/Si coaxial NW heterostructure, which yielded photocurrent density up to 15 mA/cm2 （at 0 V vs. the reversible hydrogen electrode （RHE）） with goo stability under the operating conditions employed. This work reveals the earth-abundant electrocatalysts coupled with high surface area NW electrod~ can provide performance comparable to noble metal catalysts for photocathod hydrogen evolution.
