Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess electricity.Cu is the only single metal catalyst that can electrochemically convert CO2 into multicarbon product...Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess electricity.Cu is the only single metal catalyst that can electrochemically convert CO2 into multicarbon products.However,Cu exhibits an unfavorable activity and selectivity for the generation of C2 products because of the insufficient amount of CO*provided for the C‐C coupling.Based on the strong CO2 adsorption and ultrafast reaction kinetics of CO*formation on Pd,an intimate CuPd(100)interface was designed to lower the intermediate reaction barriers and improve the efficiency of C2 product formation.Density functional theory(DFT)calculations showed that the CuPd(100)interface enhanced the CO2 adsorption and decreased the CO2*hydrogenation energy barrier,which was beneficial for the C‐C coupling.The potential‐determining step(PDS)barrier of CO2 to C2 products on the CuPd(100)interface was 0.61 eV,which was lower than that on Cu(100)(0.72 eV).Encouraged by the DFT calculation results,the CuPd(100)interface catalyst was prepared by a facile chemical solution method and characterized by transmission electron microscopy.CO2 temperature‐programmed desorption and gas sensor experiments further confirmed the enhancement of the CO2 adsorption and CO2*hydrogenation ability of the CuPd(100)interface catalyst.Specifically,the obtained CuPd(100)interface catalyst exhibited a C2 Faradaic efficiency of 50.3%±1.2%at‒1.4 VRHE in 0.1 M KHCO3,which was 2.1 times higher than that of the Cu catalyst(23.6%±1.5%).This study provides the basis for the rational design of Cu‐based electrocatalysts for the generation of multicarbon products by fine‐tuning the intermediate reaction barriers.展开更多
This work focuses on the characteristics of the Rayleigh-Taylor Instability （RTI） of the interfaces formed by two semi-infinitely distributed fluids and one interlayer. In consideration of the coupling effects betwe...This work focuses on the characteristics of the Rayleigh-Taylor Instability （RTI） of the interfaces formed by two semi-infinitely distributed fluids and one interlayer. In consideration of the coupling effects between the interfaces, the expression of the growth rate is obtained. The result reveals that the instability growth rate depends on the density and thickness of the interlayer. It is found that /f the interlayer thickness is less than 0.6 times of the disturbing wavelength, the coupling effects should be considered.展开更多
文摘Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess electricity.Cu is the only single metal catalyst that can electrochemically convert CO2 into multicarbon products.However,Cu exhibits an unfavorable activity and selectivity for the generation of C2 products because of the insufficient amount of CO*provided for the C‐C coupling.Based on the strong CO2 adsorption and ultrafast reaction kinetics of CO*formation on Pd,an intimate CuPd(100)interface was designed to lower the intermediate reaction barriers and improve the efficiency of C2 product formation.Density functional theory(DFT)calculations showed that the CuPd(100)interface enhanced the CO2 adsorption and decreased the CO2*hydrogenation energy barrier,which was beneficial for the C‐C coupling.The potential‐determining step(PDS)barrier of CO2 to C2 products on the CuPd(100)interface was 0.61 eV,which was lower than that on Cu(100)(0.72 eV).Encouraged by the DFT calculation results,the CuPd(100)interface catalyst was prepared by a facile chemical solution method and characterized by transmission electron microscopy.CO2 temperature‐programmed desorption and gas sensor experiments further confirmed the enhancement of the CO2 adsorption and CO2*hydrogenation ability of the CuPd(100)interface catalyst.Specifically,the obtained CuPd(100)interface catalyst exhibited a C2 Faradaic efficiency of 50.3%±1.2%at‒1.4 VRHE in 0.1 M KHCO3,which was 2.1 times higher than that of the Cu catalyst(23.6%±1.5%).This study provides the basis for the rational design of Cu‐based electrocatalysts for the generation of multicarbon products by fine‐tuning the intermediate reaction barriers.
文摘将双核金属酞菁衍生物添加到羧甲基纤维素阳膜层制备改性的羧甲基纤维素/壳聚糖双极膜(CMC/CS BPM),用扫描电子显微镜(SEM),电子万能试验机等对其进行了表征。结果表明改性后膜的离子交换容量和双极膜的机械性能得到提高,双极膜的溶胀度下降.此外,具有不同中心金属离子的双核金属酞菁衍生物较具相同中心金属离子的双核酞菁衍生物有更强催化中间界面层水解离能力.当电流密度为60 mA.cm-2时,FeCoPc2(COOH)12改性的双极膜槽电压只有5.3 V.
文摘分别用Fe3+和戊二醛作为交联剂对羧甲基纤维素钠(CMC)-聚乙烯醇(PVA)阳膜层和壳聚糖(CS)-聚乙烯醇阴膜层进行改性,在中间界面层引入以静电纺丝技术制备的聚丙烯腈(PAN)-四磺酸基铜酞菁(CuTsPc)纳米纤维纺丝,制备了CMC-PVA/PAN-CuTsPc/CS-PVA双极膜(BPM).并用扫描电镜、接触角测定仪,电流密度-槽电压关系曲线、交流阻抗谱等对制备的双极膜进行了表征.结果表明,CMC-PVA阳膜用PAN-CuTsPc纳米纤维纺丝改性后,表面亲水性增强,中间界面层水解离效率提高,致使双极膜的膜阻抗和IR降显著降低.CMC-PVA/PAN-CuTsPc/CS-PVA(w(CuTsPc):3.0%)双极膜在90 mA·cm-2电流密度时的电阻压降(即膜IR降)仅为0.9 V.
基金Supported by National Natural Science Foundation of China under Grant No.11074300National Basic Research Program of China under Grant No.2013CBA01504+1 种基金National Science and Technology Major Project of the Ministry of ScienceTechnology of China under Grant No.2011ZX05038-001
文摘This work focuses on the characteristics of the Rayleigh-Taylor Instability （RTI） of the interfaces formed by two semi-infinitely distributed fluids and one interlayer. In consideration of the coupling effects between the interfaces, the expression of the growth rate is obtained. The result reveals that the instability growth rate depends on the density and thickness of the interlayer. It is found that /f the interlayer thickness is less than 0.6 times of the disturbing wavelength, the coupling effects should be considered.
