For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is ch...For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.展开更多
Two-dimensional metal–organic frameworks(2D MOFs),as a new type of 2D materials,have been widely applied in various applications because of their unique structures and exposed active sites.Herein,we reported two low-...Two-dimensional metal–organic frameworks(2D MOFs),as a new type of 2D materials,have been widely applied in various applications because of their unique structures and exposed active sites.Herein,we reported two low-cost 2D MOFs constructed by a raw chemical succinic acid(SA),M-SA(M=Ni or Co),which served as efficient photocatalysts for the reduction of CO_(2)to CO.Taking advantage of the thinness and open metal sites,the ultrathin Ni-SA nanosheets(ca.3.6 nm)exhibited excellent CO production of 6.96(7)mmol·g^(−1)·h^(−1)and CO selectivity of 96.6%.Photoelectrochemical tests and theoretical calculations further confirmed the higher charge transfer efficiency and unsaturated metal sites for promoting photocatalytic performances.More importantly,Ni-SA can also be synthesized in large-scale by an energy-saving method under room temperature,strongly suggesting its promising future and potential for practical applications.展开更多
Alkali and alkaline ion substitutions enhance the electrochemical properties of P2 sodium layered oxide,while the effect on electrochemical property enhancement of alkali and alkaline ions co-substitution is still unc...Alkali and alkaline ion substitutions enhance the electrochemical properties of P2 sodium layered oxide,while the effect on electrochemical property enhancement of alkali and alkaline ions co-substitution is still unclear.In this work,the structural and electrochemical properties of the Li alkali and Mg alkaline ions co-substituted P2 layered oxide Na_(0.67)(Li_(0.5)Mg_(0.5))_(0.1)(Ni_(0.33)Mn_(0.67))_(0.9)O_(2)are investigated in detail.Compared to the pristine and single-ion substituted materials,the co-substituted material shows an enhanced cycling performance with a reversible ca-pacity of 127 mAh/g and a capacity retention of 75%over 100 cycles at 0.5C.Galvanostatic intermittent titration technique(GITT)and cyclic voltammetry(CV)results show that the Li and Mg synergistically improve the ion diffusion.Moreover,the structure stability is also improved by the Li and Mg co-substitution that is clarified by operando X-ray diffraction(XRD)measurements.These results explain the origin of the enhanced electrochemical properties of the Li/Mg co-substituted P2 layered oxides for sodium ion batteries.展开更多
Cu-based materials are seldom reported as oxygen evolution reaction(OER)electrocatalysts due to their inherent electron orbital configuration,which makes them difficult to adsorb oxygen-intermediates during OER.Reason...Cu-based materials are seldom reported as oxygen evolution reaction(OER)electrocatalysts due to their inherent electron orbital configuration,which makes them difficult to adsorb oxygen-intermediates during OER.Reasonably engineering the hierarchical architectures and the electronic structures can improve the performance of Cu-based OER catalysts,such as constructing multilevel morphology,inducing the porous materials,improving the Cu valence,building heterostructures,doping heteroatoms,etc.In this work,copper-1,3,5-benzenetricarboxylate(HKUST-1)octahedra in-situ grow on the Cu nanorod(NR)-supported N-doped carbon microplates,meanwhile an active layer of Cu(OH)_(2)forms on the surface of the original conductive Cu NRs.The octahedral HKUST-1,serving as a spacer between the microplates,greatly improves the porosity and increases the available active sites,facilitating the mass transport and electron transfer,thus resulting in greatly enhanced OER performance.展开更多
基金The authors acknowledge the financial support from the Natural Science Foundation of China(Nos.21931002 and 22101123)the National Key Research and Development Program of China(2018YFB0704100)+4 种基金the Shenzhen Science and Technology Innovation Committee(no.JCYJ20200109140812302)the Leading talents of Guangdong province program(2016LJ06N507)the Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(no.2018B030322001)the Guangdong Provincial Key Laboratory of Catalysis(no.2020B121201002)Outstanding Talents Training Fund in Shenzhen.
文摘For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.
基金Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM)(No.ZDSYS20210709112802010)China Postdoctoral Science Foundation(No.2022M711483).
文摘Two-dimensional metal–organic frameworks(2D MOFs),as a new type of 2D materials,have been widely applied in various applications because of their unique structures and exposed active sites.Herein,we reported two low-cost 2D MOFs constructed by a raw chemical succinic acid(SA),M-SA(M=Ni or Co),which served as efficient photocatalysts for the reduction of CO_(2)to CO.Taking advantage of the thinness and open metal sites,the ultrathin Ni-SA nanosheets(ca.3.6 nm)exhibited excellent CO production of 6.96(7)mmol·g^(−1)·h^(−1)and CO selectivity of 96.6%.Photoelectrochemical tests and theoretical calculations further confirmed the higher charge transfer efficiency and unsaturated metal sites for promoting photocatalytic performances.More importantly,Ni-SA can also be synthesized in large-scale by an energy-saving method under room temperature,strongly suggesting its promising future and potential for practical applications.
基金supported by Guangdong Basic and Applied Basic Research Foundation(2019A1515110897 and 2019B1515120028)supported by Ministry of Higher Education of Malaysia for the Fundamental Research Grant(FRGS/1/2018/STG02/UM/02/10)awarded to Woo Haw JiunnUniversity of Malaya research grant(GPF 038B-2018)
文摘Alkali and alkaline ion substitutions enhance the electrochemical properties of P2 sodium layered oxide,while the effect on electrochemical property enhancement of alkali and alkaline ions co-substitution is still unclear.In this work,the structural and electrochemical properties of the Li alkali and Mg alkaline ions co-substituted P2 layered oxide Na_(0.67)(Li_(0.5)Mg_(0.5))_(0.1)(Ni_(0.33)Mn_(0.67))_(0.9)O_(2)are investigated in detail.Compared to the pristine and single-ion substituted materials,the co-substituted material shows an enhanced cycling performance with a reversible ca-pacity of 127 mAh/g and a capacity retention of 75%over 100 cycles at 0.5C.Galvanostatic intermittent titration technique(GITT)and cyclic voltammetry(CV)results show that the Li and Mg synergistically improve the ion diffusion.Moreover,the structure stability is also improved by the Li and Mg co-substitution that is clarified by operando X-ray diffraction(XRD)measurements.These results explain the origin of the enhanced electrochemical properties of the Li/Mg co-substituted P2 layered oxides for sodium ion batteries.
基金the National Natural Science Foundation of China(Nos.U1904215 and 21875207)the Natural Science Foundation of Jiangsu Province(No.BK20200044)the Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM,No.ZDSYS20210709112802010).
文摘Cu-based materials are seldom reported as oxygen evolution reaction(OER)electrocatalysts due to their inherent electron orbital configuration,which makes them difficult to adsorb oxygen-intermediates during OER.Reasonably engineering the hierarchical architectures and the electronic structures can improve the performance of Cu-based OER catalysts,such as constructing multilevel morphology,inducing the porous materials,improving the Cu valence,building heterostructures,doping heteroatoms,etc.In this work,copper-1,3,5-benzenetricarboxylate(HKUST-1)octahedra in-situ grow on the Cu nanorod(NR)-supported N-doped carbon microplates,meanwhile an active layer of Cu(OH)_(2)forms on the surface of the original conductive Cu NRs.The octahedral HKUST-1,serving as a spacer between the microplates,greatly improves the porosity and increases the available active sites,facilitating the mass transport and electron transfer,thus resulting in greatly enhanced OER performance.