Ammonia(NH_(3))is considered as one of the essential feedstocks in the fertilizer and chemical industries,serving as an ideal zero-carbon energy carrier.The ammonia synthesis process relies on Haber-Bosch process,prim...Ammonia(NH_(3))is considered as one of the essential feedstocks in the fertilizer and chemical industries,serving as an ideal zero-carbon energy carrier.The ammonia synthesis process relies on Haber-Bosch process,primarily involving the reaction between hydrogen(H_(2))and nitrogen(N_(2))at temperatures ranging from 400 to 500℃ and pressures exceeding 100 bar.A global total of 180 million metric tons of ammonia were produced annually in centralized industrial plants through the Haber-Bosch process,which consumes roughly 1% of the global energy supply and contributes over 1.3% of global carbon dioxide emissions[1].展开更多
Currently,the energy and capital intensive Haber–Bosch process still dominates NH_(3)synthesis which operates at high temperatures and pressures releasing inevitably large amounts of CO_(2).The electrocatalytic N_(2)...Currently,the energy and capital intensive Haber–Bosch process still dominates NH_(3)synthesis which operates at high temperatures and pressures releasing inevitably large amounts of CO_(2).The electrocatalytic N_(2)reduction reaction(NRR)offers us an environmentally-friendly and sustainable route for NH_(3)synthesis under ambient conditions.展开更多
The Haber Bosch industrial NH_(3) production process has high energy consumption and severe CO_(2) emission.Electrochemical N_(2) reduction is an attractive method for the synthesis of carbon-neutral NH_(3).However,si...The Haber Bosch industrial NH_(3) production process has high energy consumption and severe CO_(2) emission.Electrochemical N_(2) reduction is an attractive method for the synthesis of carbon-neutral NH_(3).However,since an efficient electrocatalyst is required to perform the N_(2) reduction reaction (NRR) at room temperature,N_(2) activation is a severe challenge.Herein,we report a CeP nanoparticle–reduced graphene oxide (CeP–rGO) hybrid as an effective electrocatalyst for NH_(3) synthesis.In 0.1 M HCl,CeP–rGO achieves a large NH_(3) yield of 28.69 μg h^(−1) mg_(cat.)^(−1) and a high faradaic efficiency of 9.6% at −0.40 V,and it also shows high electrochemical and structural stability.Density functional theory (DFT) calculations show that CeP can efficiently catalyze the synthesis of NH_(3).展开更多
Ambient ammonia synthesis via the electrochemical reduction of nitrate (NO_(3)^(-)) offers us a sustainable alternative to the industrial energy-intensive Haber–Bosch process. Here,we report on the development of NiF...Ambient ammonia synthesis via the electrochemical reduction of nitrate (NO_(3)^(-)) offers us a sustainable alternative to the industrial energy-intensive Haber–Bosch process. Here,we report on the development of NiFe_(2)O_(4) nanosheet arrays on carbon cloth (NiFe_(2)O_(4)/CC) for high-efficiency NH_(3) electrosynthesis via the selective reduction of NO_(3)^(-) under ambient conditions. When operated in 0.1 M phosphate-buffered solution with additional 0.1 M NaNO_(3),such NiFe_(2)O_(4)/CC achieves a remarkable faradaic efficiency of 96.6% and a high NH_(3) yield of up to 10.3 mg h^(-1) cm^(-2). Furthermore,it possesses excellent electrochemical and structural stability. The theoretical calculations reveal that the metallic NiFe_(2)O_(4) surface has strong interactions with NO_(3)^(-) and can seriously inhibit the HER aiding in more efficient NO_(3)^(-) reduction to NH_(3).展开更多
Traditional NH_(3) production based on the Haber–Bosch process is usually accompanied by high energy consumption and a large amount of carbon dioxide emission,which are not conducive to the realization of global carb...Traditional NH_(3) production based on the Haber–Bosch process is usually accompanied by high energy consumption and a large amount of carbon dioxide emission,which are not conducive to the realization of global carbon neutralization.Electrochemical N_(2) reduction is regarded as a clean strategy to deal with this problem.In this work,porous LiFe_(5)O_(8) nanoparticle–reduced graphene oxide (rGO) is proposed as an efficient electrocatalyst for artificial N_(2)-to-NH_(3) fixation with excellent selectivity under ambient conditions.Electrochemical tests in 0.1 M HCl show that such a hybrid achieves a high NH_(3) yield of 36.025 mg h^(-1) mg_(cat.)^(-1) and a high faradaic efficiency of 13.08% at −0.2 V vs.the reversible hydrogen electrode.Furthermore,it also exhibits structural stability.Theoretical calculations reveal that LiFe_(5)O_(8)–rGO can efficiently catalyze NH_(3) synthesis with a low energy barrier.展开更多
基金supported by the National Natural Science Foundation of China(No.22105226)the Fundamental Research Funds for the Central Universities(23CX06019A and R20220132).
文摘Ammonia(NH_(3))is considered as one of the essential feedstocks in the fertilizer and chemical industries,serving as an ideal zero-carbon energy carrier.The ammonia synthesis process relies on Haber-Bosch process,primarily involving the reaction between hydrogen(H_(2))and nitrogen(N_(2))at temperatures ranging from 400 to 500℃ and pressures exceeding 100 bar.A global total of 180 million metric tons of ammonia were produced annually in centralized industrial plants through the Haber-Bosch process,which consumes roughly 1% of the global energy supply and contributes over 1.3% of global carbon dioxide emissions[1].
基金the National Key Research and Development Program of China(No.2017YFB0307504)the National Natural Science Foundation of China(No.21506133)the Youth Foundation of Sichuan University(No.2017SCU04a08)for their support in this research.
文摘Currently,the energy and capital intensive Haber–Bosch process still dominates NH_(3)synthesis which operates at high temperatures and pressures releasing inevitably large amounts of CO_(2).The electrocatalytic N_(2)reduction reaction(NRR)offers us an environmentally-friendly and sustainable route for NH_(3)synthesis under ambient conditions.
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘The Haber Bosch industrial NH_(3) production process has high energy consumption and severe CO_(2) emission.Electrochemical N_(2) reduction is an attractive method for the synthesis of carbon-neutral NH_(3).However,since an efficient electrocatalyst is required to perform the N_(2) reduction reaction (NRR) at room temperature,N_(2) activation is a severe challenge.Herein,we report a CeP nanoparticle–reduced graphene oxide (CeP–rGO) hybrid as an effective electrocatalyst for NH_(3) synthesis.In 0.1 M HCl,CeP–rGO achieves a large NH_(3) yield of 28.69 μg h^(−1) mg_(cat.)^(−1) and a high faradaic efficiency of 9.6% at −0.40 V,and it also shows high electrochemical and structural stability.Density functional theory (DFT) calculations show that CeP can efficiently catalyze the synthesis of NH_(3).
基金supported by the National Natural Science Foundation of China(No.22072015)。
文摘Ambient ammonia synthesis via the electrochemical reduction of nitrate (NO_(3)^(-)) offers us a sustainable alternative to the industrial energy-intensive Haber–Bosch process. Here,we report on the development of NiFe_(2)O_(4) nanosheet arrays on carbon cloth (NiFe_(2)O_(4)/CC) for high-efficiency NH_(3) electrosynthesis via the selective reduction of NO_(3)^(-) under ambient conditions. When operated in 0.1 M phosphate-buffered solution with additional 0.1 M NaNO_(3),such NiFe_(2)O_(4)/CC achieves a remarkable faradaic efficiency of 96.6% and a high NH_(3) yield of up to 10.3 mg h^(-1) cm^(-2). Furthermore,it possesses excellent electrochemical and structural stability. The theoretical calculations reveal that the metallic NiFe_(2)O_(4) surface has strong interactions with NO_(3)^(-) and can seriously inhibit the HER aiding in more efficient NO_(3)^(-) reduction to NH_(3).
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘Traditional NH_(3) production based on the Haber–Bosch process is usually accompanied by high energy consumption and a large amount of carbon dioxide emission,which are not conducive to the realization of global carbon neutralization.Electrochemical N_(2) reduction is regarded as a clean strategy to deal with this problem.In this work,porous LiFe_(5)O_(8) nanoparticle–reduced graphene oxide (rGO) is proposed as an efficient electrocatalyst for artificial N_(2)-to-NH_(3) fixation with excellent selectivity under ambient conditions.Electrochemical tests in 0.1 M HCl show that such a hybrid achieves a high NH_(3) yield of 36.025 mg h^(-1) mg_(cat.)^(-1) and a high faradaic efficiency of 13.08% at −0.2 V vs.the reversible hydrogen electrode.Furthermore,it also exhibits structural stability.Theoretical calculations reveal that LiFe_(5)O_(8)–rGO can efficiently catalyze NH_(3) synthesis with a low energy barrier.
