The kinetics of SnS evaporation from SnS-Cu2S melts was investigated by a unique experimental method. It is shown that the process is controlled by the mass transport of SnS in gas phase. The evaporation rate of SnS i...The kinetics of SnS evaporation from SnS-Cu2S melts was investigated by a unique experimental method. It is shown that the process is controlled by the mass transport of SnS in gas phase. The evaporation rate of SnS is significantly enhanced by increasing tempeature and carrier gas flow rate. The apparent activation energy for the process is found to be 204.67 kJ. The evaporation rate for the present system is much smaller than that for SnS-FeS system.展开更多
SnS has emerged as an attractive catalyst for the electrochemical CO_(2)reduction reaction(CO_(2)RR)to formate,while its long-term operational stability is hindered by the self-reduction of Sn^(2+) and sulfur dissolut...SnS has emerged as an attractive catalyst for the electrochemical CO_(2)reduction reaction(CO_(2)RR)to formate,while its long-term operational stability is hindered by the self-reduction of Sn^(2+) and sulfur dissolution.Thus,maintaining high current efficiency across a wide negative potential range to achieve high production rates of formate remains a significant challenge.In this study,we present a heterostructure constructed with SnS and CuS for efficient CO_(2)RR to formate.The SnS-CuS(30)exhibits a remarkable formate Faradaic efficiency(FE_(f))of 93.94%at−1 V vs.reversible hydrogen electrode(RHE)and demonstrates long-term stability for 7.5 h,maintaining high activity(with an average FE_(f)of 85.6%)across a wide negative potential range(from-0.8 to-1.2 V(vs.RHE)).The results reveal that the heterogeneous interface between SnS and CuS mitigates the self-reduction issue of SnS by sacrificing Cu^(2+),highlighting that the true active species is SnS,which effectively resists structural changes during the electrolysis process under the protection of CuS.The synergistic interaction within the CuS and SnS heterostructure,combined with the tendency for electron self-conduction,enables the catalyst to maintain high formate activity and selectivity across a wide potential range.Furthermore,theoretical results further indicate that the incorporation of CuS enhances CO_(2)adsorption and lowers the energy barrier for the formation of formate intermediates.This study inspires the concept of applying protective layers to active species,promoting high selectivity in Sn-based electrocatalysts.展开更多
文摘The kinetics of SnS evaporation from SnS-Cu2S melts was investigated by a unique experimental method. It is shown that the process is controlled by the mass transport of SnS in gas phase. The evaporation rate of SnS is significantly enhanced by increasing tempeature and carrier gas flow rate. The apparent activation energy for the process is found to be 204.67 kJ. The evaporation rate for the present system is much smaller than that for SnS-FeS system.
基金supported by the National Key Research and Development Program of China(No.2018YFB1501405)the National Natural Science Foundation of China(No.52476185).
文摘SnS has emerged as an attractive catalyst for the electrochemical CO_(2)reduction reaction(CO_(2)RR)to formate,while its long-term operational stability is hindered by the self-reduction of Sn^(2+) and sulfur dissolution.Thus,maintaining high current efficiency across a wide negative potential range to achieve high production rates of formate remains a significant challenge.In this study,we present a heterostructure constructed with SnS and CuS for efficient CO_(2)RR to formate.The SnS-CuS(30)exhibits a remarkable formate Faradaic efficiency(FE_(f))of 93.94%at−1 V vs.reversible hydrogen electrode(RHE)and demonstrates long-term stability for 7.5 h,maintaining high activity(with an average FE_(f)of 85.6%)across a wide negative potential range(from-0.8 to-1.2 V(vs.RHE)).The results reveal that the heterogeneous interface between SnS and CuS mitigates the self-reduction issue of SnS by sacrificing Cu^(2+),highlighting that the true active species is SnS,which effectively resists structural changes during the electrolysis process under the protection of CuS.The synergistic interaction within the CuS and SnS heterostructure,combined with the tendency for electron self-conduction,enables the catalyst to maintain high formate activity and selectivity across a wide potential range.Furthermore,theoretical results further indicate that the incorporation of CuS enhances CO_(2)adsorption and lowers the energy barrier for the formation of formate intermediates.This study inspires the concept of applying protective layers to active species,promoting high selectivity in Sn-based electrocatalysts.
