Since the successful exfoliation of graphene in 2014,twodimensional(2D)materials have explosively increased in the past few years[1].2D pnictogen materials with intriguing properties beyond graphene are gradually comi...Since the successful exfoliation of graphene in 2014,twodimensional(2D)materials have explosively increased in the past few years[1].2D pnictogen materials with intriguing properties beyond graphene are gradually coming into eyesight,such as black phosphorous(BP)[2],arsenene[3],antimonene[4],bismuthine[5],etc.BP is a star material in 2D materials.展开更多
Graphene has raised a huge wave in 2D materials field,breeding lots of graphene analogs with applications in optical and electrical devices,energy conversion and storage,bio-logy,etc.[1,2].Graphene presents superior c...Graphene has raised a huge wave in 2D materials field,breeding lots of graphene analogs with applications in optical and electrical devices,energy conversion and storage,bio-logy,etc.[1,2].Graphene presents superior carrier mobility,while its zero-bandgap restricts its transistor application.To make up this shortcoming,new 2D materials with certain bandgaps and high carrier mobility are being developed.Two typical materials are transition metal dichalcogenides(TMDs)and black phosphorus,which exhibit layered structure,layer-dependent band structure and strong quantum con-straints[3−5].As a congener of phosphorus,arsenic can complement the bandgap of existed 2D materials[6−18].展开更多
All-inorganic perovskites,adopting cesium(Cs+)cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites,have attracted much attention owing to the excellent thermal ...All-inorganic perovskites,adopting cesium(Cs+)cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites,have attracted much attention owing to the excellent thermal stability.However,all-inorganic iodine-based perovskites generally exhibit poor phase stability in ambient conditions.Herein,we propose an efficient strategy to introduce antimony(Sb^(3+))into the crystalline lattices of CsPbI_(2)Br perovskite,which can effectively regulate the growth of perovskite crystals to obtain a more stable perovskite phase.Due to the much smaller ionic radius and lower electronegativity of trivalent Sb^(3+)than those of Pb^(2+),the Sb^(3+)doping can decrease surface defects and suppress charge recombination,resulting in longer carrier lifetime and negligible hysteresis.As a result,the all-inorganic perovskite solar cells(PSCs)based on 0.25%Sb^(3+)doped CsPbI_(2)Br light absorber and screen-printable nanocarbon counter electrode achieved a power conversion efficiency of 11.06%,which is 16%higher than that of the control devices without Sb^(3+)doping.Moreover,the Sb^(3+)doped all-inorganic PSCs also exhibited greatly improved endurance against heat and moisture.Due to the use of low-cost and easy-to-process nanocarbon counter electrodes,the manufacturing process of the all-inorganic PSCs is very convenient and highly repeatable,and the manufacturing cost can be greatly reduced.This work offers a promising approach to constructing high-stability all-inorganic PSCs by introducing appropriate lattice doping.展开更多
The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and chemicals.However,its advancement is impeded by the absence of electrocatalysts with both high selectivity and stability.H...The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and chemicals.However,its advancement is impeded by the absence of electrocatalysts with both high selectivity and stability.Here,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio structure.The resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction intermediates.Benefiting from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V vs.reversible hydrogen electrode(RHE)in H-cell.Under an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(vs.RHE)and a good long-term stability for formate production.Furthermore,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms catalyst.Our results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.展开更多
Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious co...Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious constraint for the further development of perovskite solar cells(PSCs).In particular,the rapid crystallization guided by anti-solvents leads to plenty of surficial and interfacial defects in perovskite films.Herein,we report the adoption of a pseudo-halide anion based ionic liquid additive,1-butyl-3-methylimidazolium thiocyanate(BMIMSCN)for growing ternary cation(CsFAMA,where FA=formamidinium and MA=methylammonium)perovskites with large-scale crystal grains and strong preferential orientation via the enhanced Ostwald ripening.Meanwhile,a novel halide-free passivator,benzylammonium formate(BAFa),was employed as a buffering layer on the perovskite films to suppress surface-dominated charge recombination.As a result,the cooperative effects of BMIMSCN additive and BAFa passivator lead to significant enhancements on fluorescence lifetime(from 79.41 to 201.01 ns),open-circuit voltage(from 1.13 to 1.19 V),photoelectric conversion efficiency(from 18.90%to 22.33%).Moreover,the BMIMSCN/BAFa-CsFAMA PSCs demonstrated greatly improved stability against moisture and heat.This work suggests a promising strategy to improve the quality of perovskite materials via reducing the surficial and interfacial defects by the synergistic effects of lattice doping and interface engineering.展开更多
Phosphorene,especially black phosphorus(BP),has attracted considerable attention due to the unique characteristics,such as tunable direct bandgap,high carrier mobility,and strong in-plane anisotropy.Recently,a new mod...Phosphorene,especially black phosphorus(BP),has attracted considerable attention due to the unique characteristics,such as tunable direct bandgap,high carrier mobility,and strong in-plane anisotropy.Recently,a new modification strategy for black phosphorus has been developed by alloying black phosphorus with the congener element arsenic.The elemental composition tuning of black phosphorus with arsenic can not only maintain its special crystal structure and high anisotropy but also modify its electrical and optical properties for the further applications of multifunctional devices.The achieved two-dimensional(2D)black arsenic-phosphorus materials exhibit outstanding optical,electrical,and photoelectric properties,such as very narrow band gap,anisotropic infrared absorption,and bipolar transfer characteristics,presenting great potential in infrared photodetectors and highperformance field effect transistors(FETs).In this review,we introduce the recent progress made in the synthesis and applications of black arsenic-phosphorus,and provide an outlook and perspectives on the current challenges and future opportunities in this field.We hope that this review can bring new insights and inspirations on the further development of 2D black arsenic-phosphorus based materials and devices.展开更多
基金the National Natural Science Foundation of China(22022505 and 21872069)the Fundamental Research Funds for the Central Universities of China(020514380266,020514380272,and 020514380274)+5 种基金the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220008)the Scientific and Technological Achievements Transformation Special Fund of Jiangsu Province(BA2023037)the International Collaboration Research Program of Nanjing City(202201007 and 2022SX00000955)the Gusu Leading Talent Program of Scientific and Technological Innovation and Entrepreneurship of Wujiang District in Suzhou City(ZXL2021273)the National Key Research and Development Program of China(2022YFB3803300,2023YFE0116800)Beijing Natural Science Foundation(IS23037).
文摘Since the successful exfoliation of graphene in 2014,twodimensional(2D)materials have explosively increased in the past few years[1].2D pnictogen materials with intriguing properties beyond graphene are gradually coming into eyesight,such as black phosphorous(BP)[2],arsenene[3],antimonene[4],bismuthine[5],etc.BP is a star material in 2D materials.
基金the National Key Research and Development Program of China(2017YFA0208200)the Fundamental Research Funds for the Central Universities of China(0205-14380266)+4 种基金the National Natural Science Foundation of China(22022505 and 21872069)the Natural Science Foundation of Jiangsu Province(BK20180008)the Shenzhen Fundamental Research Program of Science,Technology and Innovation(JCYJ20180307155007589)the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(51773045,21772030,51922032,21961160720)for financial support.
文摘Graphene has raised a huge wave in 2D materials field,breeding lots of graphene analogs with applications in optical and electrical devices,energy conversion and storage,bio-logy,etc.[1,2].Graphene presents superior carrier mobility,while its zero-bandgap restricts its transistor application.To make up this shortcoming,new 2D materials with certain bandgaps and high carrier mobility are being developed.Two typical materials are transition metal dichalcogenides(TMDs)and black phosphorus,which exhibit layered structure,layer-dependent band structure and strong quantum con-straints[3−5].As a congener of phosphorus,arsenic can complement the bandgap of existed 2D materials[6−18].
基金support of the National Key R&D Program of China(No.2017YFA0208200)the National Natural Science Foundation of China(Nos.22022505 and 21872069)+3 种基金the Fundamental Research Funds for the Central Universities(Nos.020514380266,020514380272,and 020514380274)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(No.BK20220008)the Nanjing International Collaboration Research Program(Nos.202201007 and 2022SX00000955)the Suzhou Gusu Leading Talent Program of Science and Technology Innovation and Entrepreneurship in Wujiang District(No.ZXL2021273).
文摘All-inorganic perovskites,adopting cesium(Cs+)cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites,have attracted much attention owing to the excellent thermal stability.However,all-inorganic iodine-based perovskites generally exhibit poor phase stability in ambient conditions.Herein,we propose an efficient strategy to introduce antimony(Sb^(3+))into the crystalline lattices of CsPbI_(2)Br perovskite,which can effectively regulate the growth of perovskite crystals to obtain a more stable perovskite phase.Due to the much smaller ionic radius and lower electronegativity of trivalent Sb^(3+)than those of Pb^(2+),the Sb^(3+)doping can decrease surface defects and suppress charge recombination,resulting in longer carrier lifetime and negligible hysteresis.As a result,the all-inorganic perovskite solar cells(PSCs)based on 0.25%Sb^(3+)doped CsPbI_(2)Br light absorber and screen-printable nanocarbon counter electrode achieved a power conversion efficiency of 11.06%,which is 16%higher than that of the control devices without Sb^(3+)doping.Moreover,the Sb^(3+)doped all-inorganic PSCs also exhibited greatly improved endurance against heat and moisture.Due to the use of low-cost and easy-to-process nanocarbon counter electrodes,the manufacturing process of the all-inorganic PSCs is very convenient and highly repeatable,and the manufacturing cost can be greatly reduced.This work offers a promising approach to constructing high-stability all-inorganic PSCs by introducing appropriate lattice doping.
基金the National Key Research and Development Program of China(No.2017YFA0208200)the National Natural Science Foundation of China(Nos.22022505 and 21872069)+5 种基金the Fundamental Research Funds for the Central Universities of China(Nos.020514380266,020514380272,and 020514380274)the General Project of the Joint Fund of Equipment Pre-research and the Ministry of Education(No.8091B02052407)the Scientific and Technological Achievements Transformation Special Fund of Jiangsu Province(No.BA2023037)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(No.BK20220008)the Nanjing International Collaboration Research Program(Nos.202201007 and 2022SX00000955)the Suzhou Gusu Leading Talent Program of Science and Technology Innovation and Entrepreneurship in Wujiang District(No.ZXL2021273).
文摘The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and chemicals.However,its advancement is impeded by the absence of electrocatalysts with both high selectivity and stability.Here,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio structure.The resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction intermediates.Benefiting from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V vs.reversible hydrogen electrode(RHE)in H-cell.Under an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(vs.RHE)and a good long-term stability for formate production.Furthermore,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms catalyst.Our results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.
基金the National Key R&D Program of China(No.2017YFA0208200)the National Natural Science Foundation of China(Nos.22022505,21872069,and 22109069)+3 种基金the Fundamental Research Funds for the Central Universities of China(Nos.020514380266,020514380272,and 020514380274)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220008)the Nanjing International Collaboration Research Program(Nos.202201007 and 2022SX00000955)the Suzhou Gusu Leading Talent Program of Science and Technology Innovation and Entrepreneurship in Wujiang District(No.ZXL2021273).
文摘Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious constraint for the further development of perovskite solar cells(PSCs).In particular,the rapid crystallization guided by anti-solvents leads to plenty of surficial and interfacial defects in perovskite films.Herein,we report the adoption of a pseudo-halide anion based ionic liquid additive,1-butyl-3-methylimidazolium thiocyanate(BMIMSCN)for growing ternary cation(CsFAMA,where FA=formamidinium and MA=methylammonium)perovskites with large-scale crystal grains and strong preferential orientation via the enhanced Ostwald ripening.Meanwhile,a novel halide-free passivator,benzylammonium formate(BAFa),was employed as a buffering layer on the perovskite films to suppress surface-dominated charge recombination.As a result,the cooperative effects of BMIMSCN additive and BAFa passivator lead to significant enhancements on fluorescence lifetime(from 79.41 to 201.01 ns),open-circuit voltage(from 1.13 to 1.19 V),photoelectric conversion efficiency(from 18.90%to 22.33%).Moreover,the BMIMSCN/BAFa-CsFAMA PSCs demonstrated greatly improved stability against moisture and heat.This work suggests a promising strategy to improve the quality of perovskite materials via reducing the surficial and interfacial defects by the synergistic effects of lattice doping and interface engineering.
基金This work was supported by the National Key Research and Development Program of China(No.2017YFA0208200)the Fundamental Research Funds for the Central Universities of China(No.0205–14380266)+3 种基金the National Natural Science Foundation of China(Nos.22022505,21872069,and 22109069)the Natural Science Foundation of Jiangsu Province(No.BK20180008)the Doctoral Innovation and Entrepreneurship Program of Jiangsu Province(No.JSSCBS20210045)the Shenzhen Fundamental Research Program of Science,Technology and Innovation Commission of Shenzhen Municipality(No.JCYJ20180307155007589).
文摘Phosphorene,especially black phosphorus(BP),has attracted considerable attention due to the unique characteristics,such as tunable direct bandgap,high carrier mobility,and strong in-plane anisotropy.Recently,a new modification strategy for black phosphorus has been developed by alloying black phosphorus with the congener element arsenic.The elemental composition tuning of black phosphorus with arsenic can not only maintain its special crystal structure and high anisotropy but also modify its electrical and optical properties for the further applications of multifunctional devices.The achieved two-dimensional(2D)black arsenic-phosphorus materials exhibit outstanding optical,electrical,and photoelectric properties,such as very narrow band gap,anisotropic infrared absorption,and bipolar transfer characteristics,presenting great potential in infrared photodetectors and highperformance field effect transistors(FETs).In this review,we introduce the recent progress made in the synthesis and applications of black arsenic-phosphorus,and provide an outlook and perspectives on the current challenges and future opportunities in this field.We hope that this review can bring new insights and inspirations on the further development of 2D black arsenic-phosphorus based materials and devices.