采用水热合成法制备了CuS_(x)催化剂,通过改变前驱体铜硫比〔n(Cu)∶n(S)〕,调控催化剂形貌和反应路径。将CuS_(x)催化剂用于温和电势下CO_(2)高效电催化还原制CO反应。采用XRD、FESEM和XPS对CuS_(x)催化剂进行了表征,探究了铜硫比对CuS...采用水热合成法制备了CuS_(x)催化剂,通过改变前驱体铜硫比〔n(Cu)∶n(S)〕,调控催化剂形貌和反应路径。将CuS_(x)催化剂用于温和电势下CO_(2)高效电催化还原制CO反应。采用XRD、FESEM和XPS对CuS_(x)催化剂进行了表征,探究了铜硫比对CuS_(x)催化剂电催化CO_(2)还原“构效关系”的影响。结果表明,铜硫比影响CuS晶体成核与生长,进而影响CuS_(x)催化剂的形貌和S空位缺陷。当铜硫比在2∶1~1∶4内变化,CuS_(x)催化剂的形貌由荷花状转化为花球状,S空位含量由20.66%提高至63.37%,CO_(2)电催化还原活性和目标产物CO选择性明显提升。由铜硫比为1∶4制备的CuS_(x)催化剂(CuS-1∶4)在0.1 mol/L的KHCO3电解液中,在–0.51 V vs.RHE(可逆氢电极)的温和电势下,CO选择性达72.67%。CuS-1∶4优异的CO_(2)还原性能归因于催化剂花球状形貌、高比表面积和气体扩散通道提供的不饱和活性位点促进了气体扩散,以及S空位缺陷对电子传递和*COOH中间体在催化剂表面吸附的强化作用。展开更多
MoS_(2)/CuS composite catalysts were successfully synthesized using a one-step hydrothermal method with sodium molybdate dihydrate,thiourea,oxalic acid,and copper nitrate trihydrate as raw materials.The hydrogen pro-d...MoS_(2)/CuS composite catalysts were successfully synthesized using a one-step hydrothermal method with sodium molybdate dihydrate,thiourea,oxalic acid,and copper nitrate trihydrate as raw materials.The hydrogen pro-duction performance of MoS_(2)/CuS prepared with different molar ratios of Mo to Cu precursors(n_(Mo)∶n_(Cu))as cathodic catalysts was investigated in the two-chamber microbial electrolytic cell(MEC).X-ray diffraction(XRD),X-ray pho-toelectron spectroscopy(XPS),scanning electron microscopy(SEM),transmission electron microscope(TEM),linear scanning voltammetry(LSV),electrochemical impedance analysis(EIS),and cyclic voltammetry(CV)were used to characterize the synthesized catalysts for testing and analyzing the hydrogen-producing performance.The results showed that the hydrogen evolution performance of MoS_(2)/CuS-20%(nMo∶nCu=5∶1)was better than that of platinum(Pt)mesh,and the hydrogen production rate of MoS_(2)/CuS-20%as a cathode in MEC was(0.2031±0.0237)m^(3)_(H_(2))·m^(-3)·d^(-1) for 72 h at an applied voltage of 0.8 V,which was slightly higher than that of Pt mesh of(0.1886±0.0134)m^(3)_(H_(2))·m^(-3)·d^(-1).The addition of a certain amount of CuS not only regulates the electron transfer ability of MoS_(2) but also increases the density of active sites.展开更多
基金National Natural Science Foundation of China (22269010)Jiangxi Provincial Natural Science Foundation (20224BAB214021)Major Research Program of Jingdezhen Ceramic Industry (2023ZDGG002)。
文摘采用水热合成法制备了CuS_(x)催化剂,通过改变前驱体铜硫比〔n(Cu)∶n(S)〕,调控催化剂形貌和反应路径。将CuS_(x)催化剂用于温和电势下CO_(2)高效电催化还原制CO反应。采用XRD、FESEM和XPS对CuS_(x)催化剂进行了表征,探究了铜硫比对CuS_(x)催化剂电催化CO_(2)还原“构效关系”的影响。结果表明,铜硫比影响CuS晶体成核与生长,进而影响CuS_(x)催化剂的形貌和S空位缺陷。当铜硫比在2∶1~1∶4内变化,CuS_(x)催化剂的形貌由荷花状转化为花球状,S空位含量由20.66%提高至63.37%,CO_(2)电催化还原活性和目标产物CO选择性明显提升。由铜硫比为1∶4制备的CuS_(x)催化剂(CuS-1∶4)在0.1 mol/L的KHCO3电解液中,在–0.51 V vs.RHE(可逆氢电极)的温和电势下,CO选择性达72.67%。CuS-1∶4优异的CO_(2)还原性能归因于催化剂花球状形貌、高比表面积和气体扩散通道提供的不饱和活性位点促进了气体扩散,以及S空位缺陷对电子传递和*COOH中间体在催化剂表面吸附的强化作用。
文摘MoS_(2)/CuS composite catalysts were successfully synthesized using a one-step hydrothermal method with sodium molybdate dihydrate,thiourea,oxalic acid,and copper nitrate trihydrate as raw materials.The hydrogen pro-duction performance of MoS_(2)/CuS prepared with different molar ratios of Mo to Cu precursors(n_(Mo)∶n_(Cu))as cathodic catalysts was investigated in the two-chamber microbial electrolytic cell(MEC).X-ray diffraction(XRD),X-ray pho-toelectron spectroscopy(XPS),scanning electron microscopy(SEM),transmission electron microscope(TEM),linear scanning voltammetry(LSV),electrochemical impedance analysis(EIS),and cyclic voltammetry(CV)were used to characterize the synthesized catalysts for testing and analyzing the hydrogen-producing performance.The results showed that the hydrogen evolution performance of MoS_(2)/CuS-20%(nMo∶nCu=5∶1)was better than that of platinum(Pt)mesh,and the hydrogen production rate of MoS_(2)/CuS-20%as a cathode in MEC was(0.2031±0.0237)m^(3)_(H_(2))·m^(-3)·d^(-1) for 72 h at an applied voltage of 0.8 V,which was slightly higher than that of Pt mesh of(0.1886±0.0134)m^(3)_(H_(2))·m^(-3)·d^(-1).The addition of a certain amount of CuS not only regulates the electron transfer ability of MoS_(2) but also increases the density of active sites.
