Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this proces...Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this process needs efficient electrocatalysts to adsorb and activate the N2, enabling the N2 reduction reaction(NRR). Herein, we report that porous LaFeO3 nanofiber with oxygen vacancies acts as an efficient NRR electrocatalyst with abundant active sites to enhance the adsorption and activation of N2. When tested in 0.1 M HCl, such electrocatalyst achieves a high Faradaic efficiency of 8.77% and a large NH3 yield rate of 18.59 μg h–1 mgcat–1.at-0.55 V versus reversible hydrogen electrode. This catalyst also shows high long-term electrochemical stability and excellent selectivity for NH3 formation. Density functional theory calculations reveal that, by introducing oxygen vacancy on LaFeO3, the subsurface metallic ions are exposed with newly localized electronic states near the Fermi level, which facilitates the adsorption and activation of N2 molecules as well as the subsequent hydrogenation reactions.展开更多
The advancement of cost-effective and selective electrocatalyst towards CO_(2) to CO conversion is crucial for renewable energy conversion and storage,thus to achieve carbon-neutral cycle in a sustainable manner.In th...The advancement of cost-effective and selective electrocatalyst towards CO_(2) to CO conversion is crucial for renewable energy conversion and storage,thus to achieve carbon-neutral cycle in a sustainable manner.In this communication,we report that CujSb decorated Cu nanowire arrays on Cu foil act as a highly active and selective electrocatalyst for CO_(2) to CO conversion.In CO_(2)-saturated 0.1 M KHCO_(3),it achieves a high Faraday efficiency(FE)of 86.5%for CO,at-0.90 V vs.reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.08:1 to 5.9:1 by adjusting the potential.It is worth noting that HCOO-product was totally suppressed on such catalyst,compared with Sb counterpart.The improving selectivity for CO could be attributed to the bimetallic effect and nanowire arrays structure.展开更多
基金the National Natural Science Foundation of China(Nos.21575137 and 11704005)。
文摘Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this process needs efficient electrocatalysts to adsorb and activate the N2, enabling the N2 reduction reaction(NRR). Herein, we report that porous LaFeO3 nanofiber with oxygen vacancies acts as an efficient NRR electrocatalyst with abundant active sites to enhance the adsorption and activation of N2. When tested in 0.1 M HCl, such electrocatalyst achieves a high Faradaic efficiency of 8.77% and a large NH3 yield rate of 18.59 μg h–1 mgcat–1.at-0.55 V versus reversible hydrogen electrode. This catalyst also shows high long-term electrochemical stability and excellent selectivity for NH3 formation. Density functional theory calculations reveal that, by introducing oxygen vacancy on LaFeO3, the subsurface metallic ions are exposed with newly localized electronic states near the Fermi level, which facilitates the adsorption and activation of N2 molecules as well as the subsequent hydrogenation reactions.
基金supported by the National Natural Science Foundation of China(No.22072015)the Foundation of Sichuan Department of Science and Technology(No.2017FZ0079).
文摘The advancement of cost-effective and selective electrocatalyst towards CO_(2) to CO conversion is crucial for renewable energy conversion and storage,thus to achieve carbon-neutral cycle in a sustainable manner.In this communication,we report that CujSb decorated Cu nanowire arrays on Cu foil act as a highly active and selective electrocatalyst for CO_(2) to CO conversion.In CO_(2)-saturated 0.1 M KHCO_(3),it achieves a high Faraday efficiency(FE)of 86.5%for CO,at-0.90 V vs.reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.08:1 to 5.9:1 by adjusting the potential.It is worth noting that HCOO-product was totally suppressed on such catalyst,compared with Sb counterpart.The improving selectivity for CO could be attributed to the bimetallic effect and nanowire arrays structure.