To perform the electrochemical nitrogen reduction reaction(NRR)under milder conditions for sustainable ammonia production,electrocatalysts should exhibit high selectivity,activity,and durability.However,the key restri...To perform the electrochemical nitrogen reduction reaction(NRR)under milder conditions for sustainable ammonia production,electrocatalysts should exhibit high selectivity,activity,and durability.However,the key restrictions are the highly stable N≡N triple bond and the competitive hydrogen evolution reaction(HER),which make it difficult to adsorb and activate N2 on the surface of electrocatalysts,leading to a low ammonia yield and Faraday efficiency.Inspired by the enzymatic nitrogenase process and using the Fe-Mo as the active center,here we report supported Fe_(2)Mo_(3)O_(8)/XC-72 as an effective and durable electrocatalyst for the NRR.Fe_(2)Mo_(3)O_(8)/XC-72 exhibited NRR activity with an NH3 yield of 30.4μg·h^(−1)·mg^(−1)(−0.3 V)and a Faraday efficiency of 8.2%(−0.3 V).Theoretical calculations demonstrated that the electrocatalytic nitrogen fixation mechanism involved the Fe atom in the Fe_(2)Mo_(3)O_(8)/XC-72 electrocatalyst acting as the main active site in the enzymatic pathway(*NH2→*NH3),which activated nitrogen molecules and promoted the NRR performance.展开更多
1 Results Pt-Ru nanoparticles are synthesised on the surface oxidized carbon Vulcane XC-72 as catalyst support by chemically anchoring Pt and Ru onto the surface of modified carbon vulcane XC-72 (by refluxing in 70% H...1 Results Pt-Ru nanoparticles are synthesised on the surface oxidized carbon Vulcane XC-72 as catalyst support by chemically anchoring Pt and Ru onto the surface of modified carbon vulcane XC-72 (by refluxing in 70% HNO3 at 120 ℃ for 12 h to introduce surface functional groups) .The nanoparticles of Pt and Ru are synthesized by reduction of H2PtCl6 and K4Ru(CN)6 with sodium borohydride in a 5.5 buffer solution of sodium citrate,the complexation of citrate with metal ions is beneficial to the formati...展开更多
1 Results Surface oxidized carbon vulcane XC-72 as catalyst support, prepared by chemically anchoring Pt onto the surface modified carbon vulcane XC-72. The nanoparticles of Pt are synthesized by reduction of H2PtCl6 ...1 Results Surface oxidized carbon vulcane XC-72 as catalyst support, prepared by chemically anchoring Pt onto the surface modified carbon vulcane XC-72. The nanoparticles of Pt are synthesized by reduction of H2PtCl6 with sodium borohydride in a 5.5 buffer solution of sodium citrate, the complexation of citrate with metal ions is beneficial to the formation of nanoparticles. For comparison, an electrode is prepared by E-Tek Pt/C 20 Wt% with a typical Pt loading of 50 μg·cm-2, that shows higher specifi...展开更多
基金support from the Beijing Municipal High Level Innovative Team Building Program(No.IDHT20180504)Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910005017)+2 种基金the National Natural Science Foundation of China(Nos.51801006,21805004,21872001,and 21936001)Beijing Natural Science Foundation(No.2192005)Beijing Municipal Science and Natural Science Fund Project(Nos.KM201910005016 and 2017000020124G085).
文摘To perform the electrochemical nitrogen reduction reaction(NRR)under milder conditions for sustainable ammonia production,electrocatalysts should exhibit high selectivity,activity,and durability.However,the key restrictions are the highly stable N≡N triple bond and the competitive hydrogen evolution reaction(HER),which make it difficult to adsorb and activate N2 on the surface of electrocatalysts,leading to a low ammonia yield and Faraday efficiency.Inspired by the enzymatic nitrogenase process and using the Fe-Mo as the active center,here we report supported Fe_(2)Mo_(3)O_(8)/XC-72 as an effective and durable electrocatalyst for the NRR.Fe_(2)Mo_(3)O_(8)/XC-72 exhibited NRR activity with an NH3 yield of 30.4μg·h^(−1)·mg^(−1)(−0.3 V)and a Faraday efficiency of 8.2%(−0.3 V).Theoretical calculations demonstrated that the electrocatalytic nitrogen fixation mechanism involved the Fe atom in the Fe_(2)Mo_(3)O_(8)/XC-72 electrocatalyst acting as the main active site in the enzymatic pathway(*NH2→*NH3),which activated nitrogen molecules and promoted the NRR performance.
文摘1 Results Pt-Ru nanoparticles are synthesised on the surface oxidized carbon Vulcane XC-72 as catalyst support by chemically anchoring Pt and Ru onto the surface of modified carbon vulcane XC-72 (by refluxing in 70% HNO3 at 120 ℃ for 12 h to introduce surface functional groups) .The nanoparticles of Pt and Ru are synthesized by reduction of H2PtCl6 and K4Ru(CN)6 with sodium borohydride in a 5.5 buffer solution of sodium citrate,the complexation of citrate with metal ions is beneficial to the formati...
文摘1 Results Surface oxidized carbon vulcane XC-72 as catalyst support, prepared by chemically anchoring Pt onto the surface modified carbon vulcane XC-72. The nanoparticles of Pt are synthesized by reduction of H2PtCl6 with sodium borohydride in a 5.5 buffer solution of sodium citrate, the complexation of citrate with metal ions is beneficial to the formation of nanoparticles. For comparison, an electrode is prepared by E-Tek Pt/C 20 Wt% with a typical Pt loading of 50 μg·cm-2, that shows higher specifi...
