Electrocatalytic reduction of nitrates plays a crucial role in ammonia(NH3)production.In this study,a novel cuprous oxide/graphdiyne(Cu2O/GDY)electrocatalyst was synthesized by growing Cu2O/GDY on a Cu substrate with ...Electrocatalytic reduction of nitrates plays a crucial role in ammonia(NH3)production.In this study,a novel cuprous oxide/graphdiyne(Cu2O/GDY)electrocatalyst was synthesized by growing Cu2O/GDY on a Cu substrate with a porous architecture capable of increasing the number of active sites and enhancing mass transfer ability.The sp-C–Cu bonds between Cu2O and GDY facilitate rapid charge transfer and promote direct electron transport from active sites to reaction intermediates.Consequently,the electrocatalyst exhibits high NH_(3)production performance with a yield rate(YNH3)of 652.82µmol h^(-1)cm^(-2)and Faradaic efficiency of 82.98%at-1.8 V(vs.SCE)under ambient conditions in an aqueous solution.This work introduces a novel and efficient approach for the in situ fabrication of self-supported heterostructures,thereby enabling high-performance ammonia production under ambient conditions.展开更多
Electrocatalytic water splitting is a green and sustainable solution for hydrogen production,but its overall performance is still limited by the sluggish and inefficient oxygen evolution reaction(OER).Here,we report t...Electrocatalytic water splitting is a green and sustainable solution for hydrogen production,but its overall performance is still limited by the sluggish and inefficient oxygen evolution reaction(OER).Here,we report the controlled growth of vanadium–iridium oxides(VIrOx)on the surface of graphdiyne(GDY)to generate well-defined interfaces between GDY and VIrOx.The scanning electron microscopy and high-resolution transmission electron microscopy images showed the successful growth and uniform distribution of VIrOx quantum dots on the surface of the GDY nanosheets.The X-ray photoelectron spectra revealed that efficient charge transfer occurred at the interfaces between GDY and VIrOx quantum dots and led to the formation of mixed-valence metal species.These catalyst advantages notably increased the number of active sites and improved the overall intrinsic activity of the system,resulting in excellent electrocatalytic OER performance with a low overpotential of 121 mV at 10 mA cm^(-2),high turnover frequency of 0.914 s^(-1)at 300 mV,and long-term stability(100 h at 100 mA cm^(–2))in alkaline electrolytes.展开更多
The oxygen evolution reaction determines the overall efficiency of hydrogen production from water electrolysis,and still faces challenges to improve its efficiency and potential for industrial applications.Herein,we h...The oxygen evolution reaction determines the overall efficiency of hydrogen production from water electrolysis,and still faces challenges to improve its efficiency and potential for industrial applications.Herein,we have achieved the controllable synthesis of a lamination structure electrocatalyst by the in-situ growing of a film of graphdiyne(GDY)on the surface of nickel sulfide(NiSx)nanosheets.Experimental results show that the grown GDY could enhance the electric conductivity,enlarge the electrocatalytic surface area and increase the number active sites,which all benefit to increase the overall intrinsic activity of the GDY/NiSx.An exciting result is that the comprehensive performance of the catalyst is excellent with low overpotentials.The grown GDY surface guarantees the high long-term stability of the electrocatalyst.展开更多
Graphdiyne(GDY)science is a new and rapidly developing interdisciplinary field that touches on various areas of chemistry,physics,information science,material science,life science,environmental science,and so on.The r...Graphdiyne(GDY)science is a new and rapidly developing interdisciplinary field that touches on various areas of chemistry,physics,information science,material science,life science,environmental science,and so on.The rapid development of GDY science is part of the trend in development of carbon materials.GDY,with its unique structure and fascinating properties,has greatly promoted fundamental research toward practical applications of carbon materials.Many important applications,such as catalysis and energy conversion,have been reported.In particular,GDY has shown great potential for application in the field of catalysis.Scientists have precisely synthesized a series of GDY-based multiscale catalysts and applied them in various energy conversion and catalysis research,including ammonia synthesis,hydrogen production,CO_(2) conversion,and chemical-to-electrical energy conversion.In this paper,we systematically review the advances in the precisely controlled synthesis of GDY and aggregated structures,and the latest progress with GDY in catalysis and energy conversion.展开更多
Atomic catalysts(ACs)have been considered as promising catalysts for efficient hydrogen production through water splitting.Herein,we report an AC with single Mn atoms highly dispersed on the surface of graphdiynecoate...Atomic catalysts(ACs)have been considered as promising catalysts for efficient hydrogen production through water splitting.Herein,we report an AC with single Mn atoms highly dispersed on the surface of graphdiynecoated copper hydroxide nanowire arrays(Mn-GDY/Cu(OH)x NWs).By anchoring Mn atoms on GDY,the specific surface area,the number of active sites,and the stability of catalyst are greatly improved.Detailed characterizations reveal that the high hydrogen and oxygen evolution reaction(HER/OER)catalytic activity of the catalyst is induced by strong incomplete charge transfer effect between the metal atoms and GDY.These advantages enable the electrocatalysts to drive a current density of 10 mA cm^(-2)at low overpotentials of 188 and 130 mV for OER and HER,respectively,together with excellent long-term stability.Remarkably,the alkaline electrolyzer using Mn-GDY/Cu(OH)x as both cathode and anode electrodes can reach 10 mA cm^(-2)only at a much low cell voltage of 1.50 V.展开更多
析氧反应(OER)是能量转换过程中重要的半反应,开发高效、稳定、低成本的析氧反应催化剂具有重要的意义.本文报道了一种简单的原位可控生长的方法,在铜双金属氢氧化物纳米片表面原位生长石墨炔薄膜,形成了新型石墨炔/金属氢氧化物异质结...析氧反应(OER)是能量转换过程中重要的半反应,开发高效、稳定、低成本的析氧反应催化剂具有重要的意义.本文报道了一种简单的原位可控生长的方法,在铜双金属氢氧化物纳米片表面原位生长石墨炔薄膜,形成了新型石墨炔/金属氢氧化物异质结界面结构,并通过改变化学组成的方法,实现对其电催化OER活性和稳定性的有效提升.研究结果显示Ni_(0.74)Cu_(0.26)LDH@GDY/NF具有最佳OER催化性能.电流密度为10 mA cm^(-2)时的过电位仅为292 mV,且具有优异的长期稳定性,比如在6000圈连续的循环测试后OER活性几乎无衰减.实验结果表明,石墨炔的引入可以有效增加活性表面积和活性位点,促进电荷转移提高导电性,且能够高效保护催化剂不被腐蚀,从而提高整体催化性能.展开更多
Graphdiyne(GDY),a novel two-dimensional(2D)carbon allotrope featuring one-atom-thick planar layers of sp andhybridized carbon network,is a rapidly rising star on the horizon of materials science.Because of its unparal...Graphdiyne(GDY),a novel two-dimensional(2D)carbon allotrope featuring one-atom-thick planar layers of sp andhybridized carbon network,is a rapidly rising star on the horizon of materials science.Because of its unparalleled structural,electronic,chemical and physical properties,it has been receiving unprecedented increases from fundamental studies to practical applications,particularly the field of energetic materials.In this review,we aim at providing an up-to-date comprehensive overview on the state-of-the-art research into GDY,from theoretical studies to the key achievements in the development of new GDY-based energetic materials for energy storage and conversion.By reviewing the state-of-the-art achievements,we aim to address the benefits and issues of GDY-based materials,as well as highlighting the existing key challenges and future opportunities in this exciting field.展开更多
The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues...The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues.Herein,a new idea has been realized for rational and selective construction of the sp-carbon-metal-carbon interface,comprised of electronic-donating triple bonds in graphdiyne and electron-withdrawing iron carbides,for a highly efficient nitrate reduction reaction.The as-prepared sp-carbon-metal-carbon interfacial structures greatly increase the charge transfer ability and electrical conductivity of the system.The proposed concept of incomplete charge transfer has demonstrated significantly high selectivity,activity,and stability in catalytic system.The catalyst exhibits high Faradaic efficiency of over>95%and a NH3 yield rate up to 205.5μmolNH_(3) cm^(-2) h^(-1) in dilute nitrate conditions without any contaminant.展开更多
Here we report an in situ assembly growth method that controls the growth of NiTCNQ on the surface of graphdiyne(GDY).The catalytic system of donor–acceptor–donor(GDY/TCNQ/Ni)structure with multiple charge transfer(...Here we report an in situ assembly growth method that controls the growth of NiTCNQ on the surface of graphdiyne(GDY).The catalytic system of donor–acceptor–donor(GDY/TCNQ/Ni)structure with multiple charge transfer(CT)was achieved by controlling the growth of NiTCNQ on the surface of GDY.Significantly,a controlled double layer interface of GDY/TCNQ/Ni was formed.This system implemented simultaneously the two elements we expected(1)an incomplete CT,and(2)the infinite distribution of active sites originating from highly asymmetric surface charge distribution.The high conductivity and typical semiconductor characteristics of the catalyst endows it with high catalytic activity.We found that an electrolytic cell consisting of the CT salt as a catalyst provided a 1.40 V ultra-small cell voltage up to 10 mA cm−2 and the outer GDY film effectively prevented the corrosion of the catalyst.Our study is the first to introduce CT complexes to a novel catalytic material platform for high selectivity of catalysts,and undoubtedly demonstrates the high selectivity,stability,and activity of such catalytic systems,which provides a new space for the development of novel conceptual catalysts.展开更多
基金supported by the National Key Research and Development Project of China(2024YFA1509403,2022YFA1204503)Basic Science Center Project of the National Natural Science Foundation of China(22388101)+1 种基金Taishan Scholars Youth Expert Program of Shandong Province(tsqn201909050)Natural Science Foundation of Shandong Province(ZR2021JQ07,ZR2024ZD02).
文摘Electrocatalytic reduction of nitrates plays a crucial role in ammonia(NH3)production.In this study,a novel cuprous oxide/graphdiyne(Cu2O/GDY)electrocatalyst was synthesized by growing Cu2O/GDY on a Cu substrate with a porous architecture capable of increasing the number of active sites and enhancing mass transfer ability.The sp-C–Cu bonds between Cu2O and GDY facilitate rapid charge transfer and promote direct electron transport from active sites to reaction intermediates.Consequently,the electrocatalyst exhibits high NH_(3)production performance with a yield rate(YNH3)of 652.82µmol h^(-1)cm^(-2)and Faradaic efficiency of 82.98%at-1.8 V(vs.SCE)under ambient conditions in an aqueous solution.This work introduces a novel and efficient approach for the in situ fabrication of self-supported heterostructures,thereby enabling high-performance ammonia production under ambient conditions.
基金supported by the Basic Science Center Project of the National Natural Science Foundation of China(22388101)the National Key Research and Development Project of China(2022YFA1204500,2022YFA1204501,2022YFA1204503,2018YFA0703501)the Key Program of the Chinese Academy of Sciences(XDPB13).
文摘Electrocatalytic water splitting is a green and sustainable solution for hydrogen production,but its overall performance is still limited by the sluggish and inefficient oxygen evolution reaction(OER).Here,we report the controlled growth of vanadium–iridium oxides(VIrOx)on the surface of graphdiyne(GDY)to generate well-defined interfaces between GDY and VIrOx.The scanning electron microscopy and high-resolution transmission electron microscopy images showed the successful growth and uniform distribution of VIrOx quantum dots on the surface of the GDY nanosheets.The X-ray photoelectron spectra revealed that efficient charge transfer occurred at the interfaces between GDY and VIrOx quantum dots and led to the formation of mixed-valence metal species.These catalyst advantages notably increased the number of active sites and improved the overall intrinsic activity of the system,resulting in excellent electrocatalytic OER performance with a low overpotential of 121 mV at 10 mA cm^(-2),high turnover frequency of 0.914 s^(-1)at 300 mV,and long-term stability(100 h at 100 mA cm^(–2))in alkaline electrolytes.
基金supported by the Basic Science Center Project of the National Natural Science Foundation of China(grant no.22388101)the National Key Research and Development Project of China(grant nos.2022YFA1204500,2022YFA1204501,2022YFA1204503,and 2018YFA0703501)the Key Program of the Chinese Academy of Sciences(grant no.XDPB13).
文摘The oxygen evolution reaction determines the overall efficiency of hydrogen production from water electrolysis,and still faces challenges to improve its efficiency and potential for industrial applications.Herein,we have achieved the controllable synthesis of a lamination structure electrocatalyst by the in-situ growing of a film of graphdiyne(GDY)on the surface of nickel sulfide(NiSx)nanosheets.Experimental results show that the grown GDY could enhance the electric conductivity,enlarge the electrocatalytic surface area and increase the number active sites,which all benefit to increase the overall intrinsic activity of the GDY/NiSx.An exciting result is that the comprehensive performance of the catalyst is excellent with low overpotentials.The grown GDY surface guarantees the high long-term stability of the electrocatalyst.
基金This work was supported by the Basic Science Center Project of the National Natural Science Foundation of China(22388101)the National Key Research and Development Project of China(2022YFA1204500,2022YFA1204501,2022YFA1204503,2018YFA0703501)the Key Program of the Chinese Academy of Sciences(XDPB13).
文摘Graphdiyne(GDY)science is a new and rapidly developing interdisciplinary field that touches on various areas of chemistry,physics,information science,material science,life science,environmental science,and so on.The rapid development of GDY science is part of the trend in development of carbon materials.GDY,with its unique structure and fascinating properties,has greatly promoted fundamental research toward practical applications of carbon materials.Many important applications,such as catalysis and energy conversion,have been reported.In particular,GDY has shown great potential for application in the field of catalysis.Scientists have precisely synthesized a series of GDY-based multiscale catalysts and applied them in various energy conversion and catalysis research,including ammonia synthesis,hydrogen production,CO_(2) conversion,and chemical-to-electrical energy conversion.In this paper,we systematically review the advances in the precisely controlled synthesis of GDY and aggregated structures,and the latest progress with GDY in catalysis and energy conversion.
基金supported by the Fundamental Research Center of Nano Toxicology Chemistry supported through the National Natural Science Foundation of China(22388101)the National Key Research and Development Project of China(2022YFA1204500,2022YFA1204501,2022YFA1204503,2018YFA0703501)+3 种基金the National Natural Science Foundation of China(22102085)the Key Program of the Chinese Academy of Sciences(XDPB13)the Natural Science Foundation of Shandong Province(ZR2021JQ07,ZR2020ZD38)the Taishan Scholars Youth Expert Program of Shandong Province(tsqn201909050).
文摘Atomic catalysts(ACs)have been considered as promising catalysts for efficient hydrogen production through water splitting.Herein,we report an AC with single Mn atoms highly dispersed on the surface of graphdiynecoated copper hydroxide nanowire arrays(Mn-GDY/Cu(OH)x NWs).By anchoring Mn atoms on GDY,the specific surface area,the number of active sites,and the stability of catalyst are greatly improved.Detailed characterizations reveal that the high hydrogen and oxygen evolution reaction(HER/OER)catalytic activity of the catalyst is induced by strong incomplete charge transfer effect between the metal atoms and GDY.These advantages enable the electrocatalysts to drive a current density of 10 mA cm^(-2)at low overpotentials of 188 and 130 mV for OER and HER,respectively,together with excellent long-term stability.Remarkably,the alkaline electrolyzer using Mn-GDY/Cu(OH)x as both cathode and anode electrodes can reach 10 mA cm^(-2)only at a much low cell voltage of 1.50 V.
文摘析氧反应(OER)是能量转换过程中重要的半反应,开发高效、稳定、低成本的析氧反应催化剂具有重要的意义.本文报道了一种简单的原位可控生长的方法,在铜双金属氢氧化物纳米片表面原位生长石墨炔薄膜,形成了新型石墨炔/金属氢氧化物异质结界面结构,并通过改变化学组成的方法,实现对其电催化OER活性和稳定性的有效提升.研究结果显示Ni_(0.74)Cu_(0.26)LDH@GDY/NF具有最佳OER催化性能.电流密度为10 mA cm^(-2)时的过电位仅为292 mV,且具有优异的长期稳定性,比如在6000圈连续的循环测试后OER活性几乎无衰减.实验结果表明,石墨炔的引入可以有效增加活性表面积和活性位点,促进电荷转移提高导电性,且能够高效保护催化剂不被腐蚀,从而提高整体催化性能.
基金supported by the National Natural Science Foundation of China(21790050,21790051)the National Key Research and Development Project of China(2016YFA0200104)the Key Program of the Chinese Academy of Sciences(QYZDY-SSWSLH015)
文摘Graphdiyne(GDY),a novel two-dimensional(2D)carbon allotrope featuring one-atom-thick planar layers of sp andhybridized carbon network,is a rapidly rising star on the horizon of materials science.Because of its unparalleled structural,electronic,chemical and physical properties,it has been receiving unprecedented increases from fundamental studies to practical applications,particularly the field of energetic materials.In this review,we aim at providing an up-to-date comprehensive overview on the state-of-the-art research into GDY,from theoretical studies to the key achievements in the development of new GDY-based energetic materials for energy storage and conversion.By reviewing the state-of-the-art achievements,we aim to address the benefits and issues of GDY-based materials,as well as highlighting the existing key challenges and future opportunities in this exciting field.
基金This research was made possible as a result of a generous grant from the National Natural Science Foundation of China(grant nos.21790050,21790051,and 22021002)the National Key Research and Development Project of China(grant no.2018YFA0703501)the Key Program of the Chinese Academy of Sciences(grant no.XDPB13).
文摘The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues.Herein,a new idea has been realized for rational and selective construction of the sp-carbon-metal-carbon interface,comprised of electronic-donating triple bonds in graphdiyne and electron-withdrawing iron carbides,for a highly efficient nitrate reduction reaction.The as-prepared sp-carbon-metal-carbon interfacial structures greatly increase the charge transfer ability and electrical conductivity of the system.The proposed concept of incomplete charge transfer has demonstrated significantly high selectivity,activity,and stability in catalytic system.The catalyst exhibits high Faradaic efficiency of over>95%and a NH3 yield rate up to 205.5μmolNH_(3) cm^(-2) h^(-1) in dilute nitrate conditions without any contaminant.
基金by a generous grant from the National Key Research and Development Project of China(no.2018YFA0703501)the National Nature Science Foundation of China(nos.21790050,21790051,and 22021002)the Key Program of the Chinese Academy of Sciences(no.XDPB13).
文摘Here we report an in situ assembly growth method that controls the growth of NiTCNQ on the surface of graphdiyne(GDY).The catalytic system of donor–acceptor–donor(GDY/TCNQ/Ni)structure with multiple charge transfer(CT)was achieved by controlling the growth of NiTCNQ on the surface of GDY.Significantly,a controlled double layer interface of GDY/TCNQ/Ni was formed.This system implemented simultaneously the two elements we expected(1)an incomplete CT,and(2)the infinite distribution of active sites originating from highly asymmetric surface charge distribution.The high conductivity and typical semiconductor characteristics of the catalyst endows it with high catalytic activity.We found that an electrolytic cell consisting of the CT salt as a catalyst provided a 1.40 V ultra-small cell voltage up to 10 mA cm−2 and the outer GDY film effectively prevented the corrosion of the catalyst.Our study is the first to introduce CT complexes to a novel catalytic material platform for high selectivity of catalysts,and undoubtedly demonstrates the high selectivity,stability,and activity of such catalytic systems,which provides a new space for the development of novel conceptual catalysts.
