By harnessing the power of MoS_(2) as a cocatalyst to enhance electron transfer and charge carrier separation,a groundbreaking two-in-one redox photocatalytic system was developed.This innovative system integrated 2D ...By harnessing the power of MoS_(2) as a cocatalyst to enhance electron transfer and charge carrier separation,a groundbreaking two-in-one redox photocatalytic system was developed.This innovative system integrated 2D MoS_(2) nanosheets onto hydrangea-like Zn_(3)In_(2)S_(6) nanosheets,forming a 2D/3D heterostructure that established a stable and intimate interface.This unique architecture significantly improved cooperative photocatalytic performance,enabling the simultaneous production of hydrogen and benzaldehyde under light irradiation≥420 nm.Notably,the system achieved remarkable yields of hydrogen(41.9 mmol g^(-1) h^(-1))and benzaldehyde(38.9 mmol g^(-1) h^(-1)),surpassing the pristine Zn_(3)In_(2)S_(6) by 22.4 times.An impressive electron-hole pair utilization rate of approximately 93%was attained,underscoring the high efficiency of this two-in-one redox system.Additionally,the targeted 10 wt%-MoS_(2) loaded Zn_(3)In_(2)S_(6)(10MZ)nanohybrids at 400 nm obtained an apparent quantum yield(AQY)value of 17.66%without sacrificial agents or noble metals.The exceptional performance was attributed to improved charge carrier separation and reduced recombination,facilitated by cocatalyst integration and evidenced via photoluminescence,photoelectrochemical and Kelvin probe force microscopy measurements.This work highlighted the critical role of two-in-one redox-functioning heterojunctions in optimizing electron-hole pair utilization,offering a promising approach for sustainable energy production and organic synthesis.By demonstrating the potential for efficient,simultaneous generation of valuable chemicals and fuels,this research paves the way for the development of next-generation photocatalytic systems.展开更多
Integrating two different catalytic active sites into one composite is a useful 2-in-1 strategy for designing high-efficient bifunctional catalysts,which can easily tailor the activity of each reaction.Hence,we adopt ...Integrating two different catalytic active sites into one composite is a useful 2-in-1 strategy for designing high-efficient bifunctional catalysts,which can easily tailor the activity of each reaction.Hence,we adopt the 2-in-1 strategy to design the metal oxyhydroxide supported on N-doped porous carbons(PA-CoFe@NPC)as the oxygen bifunctional catalyst,where NPC provides the activity for oxygen reduction reaction(ORR)while the metal oxyhydroxide is responsible for oxygen evolution reaction(OER).Results demonstrate that the PA-CoFe@NPC indeed exhibits both super ORR and OER activities.Impressively,using bifunctional PA-CoFe@NPC as the oxygen electrode,the resulting Zn-air battery exhibits outstanding charge and discharge performance with the peak power density of 156.3 mW cm^(-2),and also exhibits a long-term cycle stability with continuous cyclic charge and discharge of 170 hours that is obviously better than the 20%Pt/C+IrO_(2)based one.The 2-in-1 strategy in this work can be efficiently extended to design other bi-or multi-functional electrocatalysts.展开更多
By tactically integrating two different kinds of proton donors and acceptors into one supramolecular tecton, a new crystalline hydrogen-bonded organic framework(HOF-SXU-1) has been developed. HOF-SXU-1 features a rema...By tactically integrating two different kinds of proton donors and acceptors into one supramolecular tecton, a new crystalline hydrogen-bonded organic framework(HOF-SXU-1) has been developed. HOF-SXU-1 features a remarkable proton conductivity as high as 6.32 mS cm^(-1) and an extremely low activation energy of 0.16 eV at 160℃ under anhydrous N_(2) conditions.By contrast, under identical conditions, the organic precursors of HOF-SXU-1 only exhibit negligible proton conduction performance, demonstrating that the formation of HOF is crucial for excellent proton conduction performance.展开更多
The first part of this report describes the data reduction of non-merohedrally twinned crystals measured on Bruker and Agilent area-detector diffractometers. The image frames of methyl-2-aminopyrazine-3-carboxylate we...The first part of this report describes the data reduction of non-merohedrally twinned crystals measured on Bruker and Agilent area-detector diffractometers. The image frames of methyl-2-aminopyrazine-3-carboxylate were processed with APEX2 to furnish a set of overlapping diffraction indices that were used for solution and refinement. CrysAlisPRO was used for processing the frames of bis（diethyldicarbamato）nickel, which exists in monoclinic and tetragonal polymorphs, and in untwinned and twinned forms. In the second part, the crystal structure of [（3-formyl-4- hydroxyphenyl）methyl]triphenylphosphanium chloride was refined through the ‘HKLF 5＇（based on a combined set of diffraction indices） and PLATON（based on one set of diffraction indices） routes to give identical outcomes because the amount of overlap of the twin domains is small. For the third part, in a proof-of-concept investigation, the diffraction pattern of untwinned and twinned 4-{（E）-（4-aminophenyl）diazenyl]phenylamine was recorded simultaneously in one run; the three domains could be indexed and the crystal structure satisfactorily refined. The refinement was identical to those derived from independent measurements; the crystal structure features two independent centrosymmetric molecules, one of which is ordered and the other whole-molecule-disordered. This two-in-one run opens up the possibility that two or more crystals having different atomic compositions can be measured simultaneously if their reciprocal lattices do not overlap significantly.展开更多
Poly(ethylene oxide)(PEO)based electrolytes have garnered considerable attention in all-solid-state lithium metal batteries with superior safety and energy density,but suffer fromlow-ion conductivity and poor cycling ...Poly(ethylene oxide)(PEO)based electrolytes have garnered considerable attention in all-solid-state lithium metal batteries with superior safety and energy density,but suffer fromlow-ion conductivity and poor cycling stability.Herein,a novel in-situ functional crosslinking strategy is proposed to overcome these limitations simultaneously,where a two-in-one bis-diazirine molecule(C1)is not only used as a rigid cross-linker,but also functions as an electron-withdrawing inducer.Benefitting from such an integration of two functionalities into one cross-linker,a rigid PEO electrolyte network can be facilely constructed,while exhibiting disrupted crystallization,robust mechanical strength,loosened Li-O binding to boost the Li+transport,and anion-rich Li+coordinated structure to favor the generation of a stable LiF-rich solid electrolyte interface.As a result,a remarkable ion conductivity of 1.4×10^(−3) S cm^(−1) is achieved at 60◦C together with a Li+transference number of 0.63.And the corresponding LiFePO4||Li and NCM811||Li filled batteries present significantly improved rate performance and capacity retention cycling life compared with the pristine PEO electrolyte,highlighting the great potential of in-situ functional crosslinking for high performance all-solid-state batteries.展开更多
基金support provided by the Ministry of Higher Education Malaysia under the Xiamen University Malaysia.-Fundamental Research Grant Scheme(FRGS)(Ref no.FRGS/1/2024/TK08/XMU/02/1)supported by the PETRONAS-Academia Collaboration Dialogue(PACD 2023)grant,provided by PETRONAS Research Sdn.Bhd.(PRSB)+6 种基金the Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF)(S.22015)supported by the National Natural Science Foundation of China(Ref no:22202168)Guangdong Basic and Applied Basic Research Foundation(Ref no:2021A1515111019)the financial support from the State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University(Ref no:2023X11)supported by the Xiamen University,Embassy of the People's Republic of China in Malaysia(EENG/0045)funded by Xiamen University Malaysia Investigatorship Grant(Grant no:IENG/0038)Xiamen University Malaysia Research Fund(ICOE/0001,XMUMRF/2021-C8/IENG/0041 and XMUMRF/2025-C15/IENG/0080).
文摘By harnessing the power of MoS_(2) as a cocatalyst to enhance electron transfer and charge carrier separation,a groundbreaking two-in-one redox photocatalytic system was developed.This innovative system integrated 2D MoS_(2) nanosheets onto hydrangea-like Zn_(3)In_(2)S_(6) nanosheets,forming a 2D/3D heterostructure that established a stable and intimate interface.This unique architecture significantly improved cooperative photocatalytic performance,enabling the simultaneous production of hydrogen and benzaldehyde under light irradiation≥420 nm.Notably,the system achieved remarkable yields of hydrogen(41.9 mmol g^(-1) h^(-1))and benzaldehyde(38.9 mmol g^(-1) h^(-1)),surpassing the pristine Zn_(3)In_(2)S_(6) by 22.4 times.An impressive electron-hole pair utilization rate of approximately 93%was attained,underscoring the high efficiency of this two-in-one redox system.Additionally,the targeted 10 wt%-MoS_(2) loaded Zn_(3)In_(2)S_(6)(10MZ)nanohybrids at 400 nm obtained an apparent quantum yield(AQY)value of 17.66%without sacrificial agents or noble metals.The exceptional performance was attributed to improved charge carrier separation and reduced recombination,facilitated by cocatalyst integration and evidenced via photoluminescence,photoelectrochemical and Kelvin probe force microscopy measurements.This work highlighted the critical role of two-in-one redox-functioning heterojunctions in optimizing electron-hole pair utilization,offering a promising approach for sustainable energy production and organic synthesis.By demonstrating the potential for efficient,simultaneous generation of valuable chemicals and fuels,this research paves the way for the development of next-generation photocatalytic systems.
文摘Integrating two different catalytic active sites into one composite is a useful 2-in-1 strategy for designing high-efficient bifunctional catalysts,which can easily tailor the activity of each reaction.Hence,we adopt the 2-in-1 strategy to design the metal oxyhydroxide supported on N-doped porous carbons(PA-CoFe@NPC)as the oxygen bifunctional catalyst,where NPC provides the activity for oxygen reduction reaction(ORR)while the metal oxyhydroxide is responsible for oxygen evolution reaction(OER).Results demonstrate that the PA-CoFe@NPC indeed exhibits both super ORR and OER activities.Impressively,using bifunctional PA-CoFe@NPC as the oxygen electrode,the resulting Zn-air battery exhibits outstanding charge and discharge performance with the peak power density of 156.3 mW cm^(-2),and also exhibits a long-term cycle stability with continuous cyclic charge and discharge of 170 hours that is obviously better than the 20%Pt/C+IrO_(2)based one.The 2-in-1 strategy in this work can be efficiently extended to design other bi-or multi-functional electrocatalysts.
基金supported by the National Natural Science Foundation of China (22001154, 22271211)the Central Government Funding for Talent Promotion (231545023)+1 种基金the Youth Fund from the Department of Science and Technology of Shanxi Province (201901D211148)the Science and Technology Innovation Planning Project in Universities and Colleges of Shanxi Province (2019L0063)。
文摘By tactically integrating two different kinds of proton donors and acceptors into one supramolecular tecton, a new crystalline hydrogen-bonded organic framework(HOF-SXU-1) has been developed. HOF-SXU-1 features a remarkable proton conductivity as high as 6.32 mS cm^(-1) and an extremely low activation energy of 0.16 eV at 160℃ under anhydrous N_(2) conditions.By contrast, under identical conditions, the organic precursors of HOF-SXU-1 only exhibit negligible proton conduction performance, demonstrating that the formation of HOF is crucial for excellent proton conduction performance.
文摘The first part of this report describes the data reduction of non-merohedrally twinned crystals measured on Bruker and Agilent area-detector diffractometers. The image frames of methyl-2-aminopyrazine-3-carboxylate were processed with APEX2 to furnish a set of overlapping diffraction indices that were used for solution and refinement. CrysAlisPRO was used for processing the frames of bis（diethyldicarbamato）nickel, which exists in monoclinic and tetragonal polymorphs, and in untwinned and twinned forms. In the second part, the crystal structure of [（3-formyl-4- hydroxyphenyl）methyl]triphenylphosphanium chloride was refined through the ‘HKLF 5＇（based on a combined set of diffraction indices） and PLATON（based on one set of diffraction indices） routes to give identical outcomes because the amount of overlap of the twin domains is small. For the third part, in a proof-of-concept investigation, the diffraction pattern of untwinned and twinned 4-{（E）-（4-aminophenyl）diazenyl]phenylamine was recorded simultaneously in one run; the three domains could be indexed and the crystal structure satisfactorily refined. The refinement was identical to those derived from independent measurements; the crystal structure features two independent centrosymmetric molecules, one of which is ordered and the other whole-molecule-disordered. This two-in-one run opens up the possibility that two or more crystals having different atomic compositions can be measured simultaneously if their reciprocal lattices do not overlap significantly.
基金supported by National Natural Science Foundation of China(No.52273198)Yunnan Fundamental Research Projects(No.202301BF070001-008)+2 种基金Graduate Research Program of Yunnan University(No.KC23235310)National Key Research and Development Program of China(Nos.2022YFB3803300 and 2023YFE0116800)Beijing Natural Science Foundation(IS23037).
文摘Poly(ethylene oxide)(PEO)based electrolytes have garnered considerable attention in all-solid-state lithium metal batteries with superior safety and energy density,but suffer fromlow-ion conductivity and poor cycling stability.Herein,a novel in-situ functional crosslinking strategy is proposed to overcome these limitations simultaneously,where a two-in-one bis-diazirine molecule(C1)is not only used as a rigid cross-linker,but also functions as an electron-withdrawing inducer.Benefitting from such an integration of two functionalities into one cross-linker,a rigid PEO electrolyte network can be facilely constructed,while exhibiting disrupted crystallization,robust mechanical strength,loosened Li-O binding to boost the Li+transport,and anion-rich Li+coordinated structure to favor the generation of a stable LiF-rich solid electrolyte interface.As a result,a remarkable ion conductivity of 1.4×10^(−3) S cm^(−1) is achieved at 60◦C together with a Li+transference number of 0.63.And the corresponding LiFePO4||Li and NCM811||Li filled batteries present significantly improved rate performance and capacity retention cycling life compared with the pristine PEO electrolyte,highlighting the great potential of in-situ functional crosslinking for high performance all-solid-state batteries.
