Exploring the efficient bifunctional catalysts and binder-free electrode materials for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is receiving continuous interest.Herein,we report the fabri...Exploring the efficient bifunctional catalysts and binder-free electrode materials for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is receiving continuous interest.Herein,we report the fabrication of hierarchical copper phosphide nanoarrays(Cu_(3)P)on three-dimensional(3D)nickel foam(NF)through a template-directed synthetic strategy as electrocatalysts for overall water splitting.Specifically,the Cu_(3)P/NF electrode demonstrates a remarkably low overpotential of~331 m V to approach the current density of 50 m A cm^(-2)in the OER,and an overpotential of~115 m V to achieve-10 m A cm^(-2)current density in the HER.Meanwhile the Cu_(3)P/NF catalyst could hold a great stability for both reactions in alkaline condition,reflected in 37 h for OER and 24 h for HER of consistent galvanostatic electrolysis.As revealed by TEM,STEM and XPS characterizations,the high catalytic OER activity can be ascribed to the 3D open structure of Cu_(3)P/NF and the abundant Cu O active sites in hierarchical Cu O/Cu_(3)P/NF structure after in-situ activation.Furthermore,the overall water splitting is conducted in a two-electrode cell,which requires only a cell voltage of 1.63 V to approach 10 m A cm^(-2)with a good stability of 20 h.This protocol of Cu_(3)P/NF electrode affords a general strategy to construct hierarchically structured metal phosphides for clean energy-related application.展开更多
Zero-dimensional(0D)hybrid metal halides are under intensive investigation owing to their unique physical properties,such as the broadband emission from highly localized excitons that is promising for white-emitting l...Zero-dimensional(0D)hybrid metal halides are under intensive investigation owing to their unique physical properties,such as the broadband emission from highly localized excitons that is promising for white-emitting lighting.However,fundamental understanding of emission variations and structure–property relationships is still limited.Here,by using pressure processing,we obtain robust exciton emission in 0D(C_(9)NH_(20))_(6)Pb_(3)Br_(12) at room temperature that can survive to 80 GPa,the recorded highest value among all the hybrid metal halides.In situ experimental characterization and first-principles calculations reveal that the pressure-induced emission is mainly caused by the largely suppressed phonon-assisted nonradiative pathway.Lattice compression leads to phonon hardening,which considerably weakens the exciton–phonon interaction and thus enhances the emission.The robust emission is attributed to the unique structure of separated spring-like[Pb_(3)Br_(12)]^(6−)trimers,which leads to the outstanding stability of the optically active inorganic units.Our findings not only reveal abnormally robust emission in a 0D metal halide,but also provide new insight into the design and optimization of local structures of trimers and oligomers in lowdimensional hybrid materials.展开更多
Achieving high yield and good quality in crops is essential for human food security and health.However,there is usually disharmony between yield and quality.Seed storage protein(SSP)and starch,the predominant componen...Achieving high yield and good quality in crops is essential for human food security and health.However,there is usually disharmony between yield and quality.Seed storage protein(SSP)and starch,the predominant components in cereal grains,determine yield and quality,and their coupled synthesis causes a yield–quality trade-off.Therefore,dissection of the underlying regulatory mechanism facilitates simultaneous improvement of yield and quality.Here,we summarize current findings about the synergistic molecular machinery underpinning SSP and starch synthesis in the leading staple cereal crops,including maize,rice and wheat.We further evaluate the functional conservation and differentiation of key regulators and specify feasible research approaches to identify additional regulators and expand insights.We also present major strategies to leverage resultant information for simultaneous improvement of yield and quality by molecular breeding.Finally,future perspectives on major challenges are proposed.展开更多
基金financially supported by the Taishan Scholar Project of Shandong Province and the Fundamental Research Funds for the Central Universities(No.18CX06065A,No.20CX06022A)the Postdoctoral Research Program of Qingdao,China(No.ZX20190140)。
文摘Exploring the efficient bifunctional catalysts and binder-free electrode materials for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is receiving continuous interest.Herein,we report the fabrication of hierarchical copper phosphide nanoarrays(Cu_(3)P)on three-dimensional(3D)nickel foam(NF)through a template-directed synthetic strategy as electrocatalysts for overall water splitting.Specifically,the Cu_(3)P/NF electrode demonstrates a remarkably low overpotential of~331 m V to approach the current density of 50 m A cm^(-2)in the OER,and an overpotential of~115 m V to achieve-10 m A cm^(-2)current density in the HER.Meanwhile the Cu_(3)P/NF catalyst could hold a great stability for both reactions in alkaline condition,reflected in 37 h for OER and 24 h for HER of consistent galvanostatic electrolysis.As revealed by TEM,STEM and XPS characterizations,the high catalytic OER activity can be ascribed to the 3D open structure of Cu_(3)P/NF and the abundant Cu O active sites in hierarchical Cu O/Cu_(3)P/NF structure after in-situ activation.Furthermore,the overall water splitting is conducted in a two-electrode cell,which requires only a cell voltage of 1.63 V to approach 10 m A cm^(-2)with a good stability of 20 h.This protocol of Cu_(3)P/NF electrode affords a general strategy to construct hierarchically structured metal phosphides for clean energy-related application.
基金supported by the National Nature Science Foundation of China(NSFC)(Grant Nos.U1930401 and 51527801)support from the National Science Foundation(Grant No.DMR-1709116)+2 种基金supported by the National Science Foundation–Earth Sciences(Grant No.EAR-1634415)the Department of Energy–GeoSciences(Grant No.DE-FG02-94ER14466)partially by COMPRES under NSF Cooperative Agreement No.EAR-1606856.
文摘Zero-dimensional(0D)hybrid metal halides are under intensive investigation owing to their unique physical properties,such as the broadband emission from highly localized excitons that is promising for white-emitting lighting.However,fundamental understanding of emission variations and structure–property relationships is still limited.Here,by using pressure processing,we obtain robust exciton emission in 0D(C_(9)NH_(20))_(6)Pb_(3)Br_(12) at room temperature that can survive to 80 GPa,the recorded highest value among all the hybrid metal halides.In situ experimental characterization and first-principles calculations reveal that the pressure-induced emission is mainly caused by the largely suppressed phonon-assisted nonradiative pathway.Lattice compression leads to phonon hardening,which considerably weakens the exciton–phonon interaction and thus enhances the emission.The robust emission is attributed to the unique structure of separated spring-like[Pb_(3)Br_(12)]^(6−)trimers,which leads to the outstanding stability of the optically active inorganic units.Our findings not only reveal abnormally robust emission in a 0D metal halide,but also provide new insight into the design and optimization of local structures of trimers and oligomers in lowdimensional hybrid materials.
基金supported by Natural Science Foundation of China(32272182)National Key Research and Development Program of China(2022YFF1002904,2022YFD1201500)+1 种基金STI 2030-Major Projects(2023ZD0406903)the Science and Technology Innovation Program of Chinese Academy of Agricultural Sciences(CAAS)。
文摘Achieving high yield and good quality in crops is essential for human food security and health.However,there is usually disharmony between yield and quality.Seed storage protein(SSP)and starch,the predominant components in cereal grains,determine yield and quality,and their coupled synthesis causes a yield–quality trade-off.Therefore,dissection of the underlying regulatory mechanism facilitates simultaneous improvement of yield and quality.Here,we summarize current findings about the synergistic molecular machinery underpinning SSP and starch synthesis in the leading staple cereal crops,including maize,rice and wheat.We further evaluate the functional conservation and differentiation of key regulators and specify feasible research approaches to identify additional regulators and expand insights.We also present major strategies to leverage resultant information for simultaneous improvement of yield and quality by molecular breeding.Finally,future perspectives on major challenges are proposed.
