Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nont...Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.展开更多
Hydrogen generated by water electrolysis is considered as one of the most promising protocols to partly replace the roles of traditional fossil fuels.However,high‐performance electrocatalyst satisfied with the indust...Hydrogen generated by water electrolysis is considered as one of the most promising protocols to partly replace the roles of traditional fossil fuels.However,high‐performance electrocatalyst satisfied with the industrial requirement still faces significant challenges.Low‐temperature plasma contains numerous high‐energy ions,electrons and other reactive species,which can provide a highly reactive environment for tuning the physio‐chemical structures of catalysts through plasma milling,etching,doping and/or deposi-tion.It is well‐known that high‐temperature micro‐filaments contained in plasmas can cause some special modifications of the catalyst surface,thus effectively adjusting the physio‐chemical structure of latterly engineered compounds.Therefore,low‐temperature plasma technologies,especially the dielectric barrier discharge(DBD)and radio frequency(RF)plasmas,can be considered as a green and sustainable strategy for engineering high‐performance electrocatalysts for water splitting(hydrogen evolution reaction[HER];oxygen evolution reaction[OER]).Herein,recent progress of DBD and RF plasmas for fabricating and modifying transition metal‐based electrocatalysts(e.g.sulphide,phos-phide,selenide,oxide,hydroxide)for hydrogen evolution reaction or OER is compre-hensively reviewed,and the role of plasma is also discussed.展开更多
基金partially supported by the Australian Research Council(ARC)the National Science Fund for Distinguished Young Scholars(grant number 51925703)。
文摘Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.
基金supported by the National Natural Science Foundation of China(52177162)the National Science Fund for Distinguished Young Scholars(51925703)+1 种基金the Zhejiang Natural Science Foundations of China(LZ22E070003)the State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(LAPS22018).
文摘Hydrogen generated by water electrolysis is considered as one of the most promising protocols to partly replace the roles of traditional fossil fuels.However,high‐performance electrocatalyst satisfied with the industrial requirement still faces significant challenges.Low‐temperature plasma contains numerous high‐energy ions,electrons and other reactive species,which can provide a highly reactive environment for tuning the physio‐chemical structures of catalysts through plasma milling,etching,doping and/or deposi-tion.It is well‐known that high‐temperature micro‐filaments contained in plasmas can cause some special modifications of the catalyst surface,thus effectively adjusting the physio‐chemical structure of latterly engineered compounds.Therefore,low‐temperature plasma technologies,especially the dielectric barrier discharge(DBD)and radio frequency(RF)plasmas,can be considered as a green and sustainable strategy for engineering high‐performance electrocatalysts for water splitting(hydrogen evolution reaction[HER];oxygen evolution reaction[OER]).Herein,recent progress of DBD and RF plasmas for fabricating and modifying transition metal‐based electrocatalysts(e.g.sulphide,phos-phide,selenide,oxide,hydroxide)for hydrogen evolution reaction or OER is compre-hensively reviewed,and the role of plasma is also discussed.
