Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel S...Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.展开更多
The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia syn...The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.展开更多
Hollow B–SiO2@TiO2 composites were prepared by the wet chemical deposition method starting from TiCl4 and hollow B–SiO2 microspheres.TiO2 layers composed of anatase TiO2 nanoparticles were coated on the surfaces of ...Hollow B–SiO2@TiO2 composites were prepared by the wet chemical deposition method starting from TiCl4 and hollow B–SiO2 microspheres.TiO2 layers composed of anatase TiO2 nanoparticles were coated on the surfaces of the hollow B–SiO2 microspheres probably through the formation of Ti—O—Si and Ti—O—B bonds.A great number of—OH groups were also present at the TiO2 coating layers.The presence of Ti—O—Si bonds and Ti—O—B bonds resulted in the formation of defects in the TiO2 coating layers,which decreased the band gap of the TiO2 coating layers to ca.3.0 eV and endowed the TiO2 coating layers with visible light absorption performance.The buoyancy hollow B–SiO2@TiO2 composites exhibited high photocatalytic activities for the degradation of ammonia-nitrogen and green algae.The conversion of ammonia-nitrogen reached 65%when the degradation of ammonia-nitrogen(43 mg·L-1 at pH value of 8)was catalyzed by the B–SiO2@TiO2(100:10)composite under the simulated solar light irradiation at 35°C for 660 min.The green algae(5 mg·L-1)were almost completely degraded over the B–SiO@TiO2(100:20)photocatalyst under the visible light irradiation at 35°C for 510 min.展开更多
Preferably 20 ppm anhydrous ammonia (NH<sub>3</sub>) is proposed to be added to hydrogen fuel (H) made from renewable energy sources (green hydrogen), so that H leaks may be easily detectable by smell, but...Preferably 20 ppm anhydrous ammonia (NH<sub>3</sub>) is proposed to be added to hydrogen fuel (H) made from renewable energy sources (green hydrogen), so that H leaks may be easily detectable by smell, but not dangerously toxic. Including this odor agent, would allow H to be distributed safely in pipes, as required by law, and it would allow H to be safely stored, transported, and exported for sale, and widely commercialized. Further research is suggested to identify optimum pressure, temperature, and automated technique for injecting NH<sub>3</sub> into H, and to chart the minimum concentration needed, as a function of temperature and humidity. An application to make hypersonic H burning aircraft safer for ground maintenance crews is proposed. An ability to make, store and distribute H, made from local sources of renewable energy, would reduce a need for fossil fuels, especially in poor, remote communities, where it could improve their economy by creating an export product for sale, while reducing pollution.展开更多
绿氢-绿氨工艺是指利用可再生能源发电、电解水制氢得到的氢气为原料合成氨的工艺流程,其具有受天气条件影响、负荷波动大、工段间耦合性强的特点。为研究绿氢-绿氨工艺流程中发输变电、电解水制氢、储氢、电化学储能、合成氨等工段之...绿氢-绿氨工艺是指利用可再生能源发电、电解水制氢得到的氢气为原料合成氨的工艺流程,其具有受天气条件影响、负荷波动大、工段间耦合性强的特点。为研究绿氢-绿氨工艺流程中发输变电、电解水制氢、储氢、电化学储能、合成氨等工段之间的系统集成和协同调度方案,利用新一代流程模拟软件AVEVA Process Simulation建立了稳态-动态双模式通用型绿氢-绿氨全流程工艺模型,并通过多稳态模拟的手段分析了系统对天气变化的动态响应。结果表明,合理设计和调度储氢和储能单元不仅可以显著稳定化工生产、合理消纳可再生电力,还能稳定网电补充,提高整体经济效益。展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.22308139,52071171,52202248)Natural Science Foundation of Liaoning Province(2023-MS-140)+11 种基金Liaoning BaiQianWan Talents Program(LNBQW2018B0048)Shenyang Science and Technology Project(21-108-9-04)Young Scientific and Technological Talents Project of the Department of Education of Liaoning Province(LQN202008)Key Research Project of Department of Education of Liaoning Province(LJKZZ20220015)Foundation of State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology(MJNYSKL202301)Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(KF2023006)Anhui Province Key Laboratory of Coal Clean Conversion and High Valued Utilization,Anhui University of Technology(CHV22-05)Australian Research Council(ARC)through Future Fellowship(FT210100298,FT210100806)Discovery Project(DP220100603)Linkage Project(LP210100467,LP210200504,LP210200345,LP220100088)Industrial Transformation Training Centre(IC180100005)schemesthe Australian Government through the Cooperative Research Centres Projects(CRCPXIII000077).
文摘Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.
基金the Science and Engineering Research Board(SERB),Government of India for funding this work(Sanction No.EEQ/2021/001116)。
文摘The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.
基金Supported by the National Natural Science Foundation of China(21506078).
文摘Hollow B–SiO2@TiO2 composites were prepared by the wet chemical deposition method starting from TiCl4 and hollow B–SiO2 microspheres.TiO2 layers composed of anatase TiO2 nanoparticles were coated on the surfaces of the hollow B–SiO2 microspheres probably through the formation of Ti—O—Si and Ti—O—B bonds.A great number of—OH groups were also present at the TiO2 coating layers.The presence of Ti—O—Si bonds and Ti—O—B bonds resulted in the formation of defects in the TiO2 coating layers,which decreased the band gap of the TiO2 coating layers to ca.3.0 eV and endowed the TiO2 coating layers with visible light absorption performance.The buoyancy hollow B–SiO2@TiO2 composites exhibited high photocatalytic activities for the degradation of ammonia-nitrogen and green algae.The conversion of ammonia-nitrogen reached 65%when the degradation of ammonia-nitrogen(43 mg·L-1 at pH value of 8)was catalyzed by the B–SiO2@TiO2(100:10)composite under the simulated solar light irradiation at 35°C for 660 min.The green algae(5 mg·L-1)were almost completely degraded over the B–SiO@TiO2(100:20)photocatalyst under the visible light irradiation at 35°C for 510 min.
文摘Preferably 20 ppm anhydrous ammonia (NH<sub>3</sub>) is proposed to be added to hydrogen fuel (H) made from renewable energy sources (green hydrogen), so that H leaks may be easily detectable by smell, but not dangerously toxic. Including this odor agent, would allow H to be distributed safely in pipes, as required by law, and it would allow H to be safely stored, transported, and exported for sale, and widely commercialized. Further research is suggested to identify optimum pressure, temperature, and automated technique for injecting NH<sub>3</sub> into H, and to chart the minimum concentration needed, as a function of temperature and humidity. An application to make hypersonic H burning aircraft safer for ground maintenance crews is proposed. An ability to make, store and distribute H, made from local sources of renewable energy, would reduce a need for fossil fuels, especially in poor, remote communities, where it could improve their economy by creating an export product for sale, while reducing pollution.
文摘绿氢-绿氨工艺是指利用可再生能源发电、电解水制氢得到的氢气为原料合成氨的工艺流程,其具有受天气条件影响、负荷波动大、工段间耦合性强的特点。为研究绿氢-绿氨工艺流程中发输变电、电解水制氢、储氢、电化学储能、合成氨等工段之间的系统集成和协同调度方案,利用新一代流程模拟软件AVEVA Process Simulation建立了稳态-动态双模式通用型绿氢-绿氨全流程工艺模型,并通过多稳态模拟的手段分析了系统对天气变化的动态响应。结果表明,合理设计和调度储氢和储能单元不仅可以显著稳定化工生产、合理消纳可再生电力,还能稳定网电补充,提高整体经济效益。
