High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental sta...High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental stability,ideal outdoor readability,and low energy consumption.However,the limited intrinsic structure of inorganic materials has presented a significant challenge in achieving precise patterning/pixelation at the micron scale.Here,we successfully developed the direct photolithography for WOx nanoparticles based on in situ photo-induced ligand exchange.This strategy enabled us to achieve ultra-high resolution efficiently(line width<4μm,the best resolution for reported inorganic electrochromic materials).Additionally,the resulting device exhibited impressive electrochromic performance,such as fast response(<1 s at 0 V),high coloration efficiency(119.5 cm^(2) C^(−1)),good optical modulation(55.9%),and durability(>3600 cycles),as well as promising applications in electronic logos,pixelated displays,flexible electronics,etc.The success and advancements presented here are expected to inspire and accelerate research and development(R&D)in high-resolution non-emissive displays and other ultra-fine micro-electronics.展开更多
Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)acc...Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)accessibility results in a universal self-adaptive structural reconstruction from Cu_(2)O to Cu@CuxO composites,ending with feeding gas-dependent microstructures and catalytic performances.The CO_(2)-rich atmosphere favors reconstruction for CO_(2)RR,whereas the CO_(2)-deficient one prefers that for hydrogen evolution reaction.With the assistance of spectroscopic analysis and theoretical calculations,we uncover a CO_(2)-induced passivation behavior by identifying a reductionresistant but catalytic active Cu(I)-rich amorphous layer stabilized by*CO intermediates.Additionally,we find extra CO production is indispensable for the robust production of C2H4.An inverse correlation between durability and FECO/FEC2H4 is disclosed,suggesting that the selfstabilization process involving the absorption of*CO intermediates on Cu(I)sites is essential for durable electrolysis.Guided by this insight,we design hollow Cu_(2)O nanospheres for durable and selective CO_(2)RR electrolysis in producing C2H4.Our work recognizes the previously overlooked passivation reconstruction and self-stabilizing behavior and highlights the critical role of the local atmosphere in modulating reconstruction and catalytic processes.展开更多
Trap-assisted charge recombination is one of the primary limitationsof restricting the performance of organic solar cells. However, effectivelyreducing the presence of traps in the photoactive layer remains challengin...Trap-assisted charge recombination is one of the primary limitationsof restricting the performance of organic solar cells. However, effectivelyreducing the presence of traps in the photoactive layer remains challenging.Herein, wide bandgap polymer donor PTzBI-dF is demonstrated as an effectivemodulator for enhancing the crystallinity of the bulk heterojunction active layerscomposed of D18 derivatives blended with Y6, leading to dense and orderedmolecular packings, and thus, improves photoluminescence quenching properties.As a result, the photovoltaic devices exhibit reduced trap-assisted charge recombinationlosses, achieving an optimized power conversion efficiency of over 19%.Besides the efficiency enhancement, the devices comprised of PTzBI-dF as athird component simultaneously attain decreased current leakage, improved chargecarrier mobilities, and suppressed bimolecular charge recombination, leading toreduced energy losses. The advanced crystalline structures induced by PTzBI-dFand its characteristics, such as well-aligned energy level, and complementaryabsorption spectra, are ascribed to the promising performance improvements.Our findings suggest that donor phase engineering is a feasible approach to tuning the molecular packings in the active layer, providingguidelines for designing effective morphology modulators for high-performance organic solar cells.展开更多
The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design platform.High-throughput screening of catalytic performance is feasible since the large MOF str...The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design platform.High-throughput screening of catalytic performance is feasible since the large MOF structure database is available.In this study,we report a machine learning model for high-throughput screening of MOF catalysts for the CO_(2) cycloaddition reaction.The descriptors for model training were judiciously chosen according to the reaction mechanism,which leads to high accuracy up to 97%for the 75%quantile of the training set as the classification criterion.The feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding.12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100℃ and 1 bar within one day using the model,and 239 potentially efficient catalysts were discovered.Among them,MOF-76(Y)achieved the top performance experimentally among reported MOFs,in good agreement with the prediction.展开更多
基金supported by the National Key R&D Program of China(2022YFB3606501,2022YFB3602902)the Key projects of National Natural Science Foundation of China(62234004)+8 种基金the National Natural Science Foundation of China(U23A2092)Pioneer and Leading Goose R&D Program of Zhejiang(2024C01191,2024C01092)Innovation and Entrepreneurship Team of Zhejiang Province(2021R01003)Ningbo Key Technologies R&D Program(2022Z085),Ningbo 3315 Programme(2020A-01-B)YONGJIANG Talent Introduction Programme(2021A-038-B,2021A-159-G)“Innovation Yongjiang 2035”Key R&D Programme(2024Z146)Ningbo JiangBei District public welfare science and technology project(2022C07)the China National Postdoctoral Program for Innovative Talents(grant no.BX20240391)the China Postdoctoral Science Foundation(grant no.2023M743623).
文摘High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental stability,ideal outdoor readability,and low energy consumption.However,the limited intrinsic structure of inorganic materials has presented a significant challenge in achieving precise patterning/pixelation at the micron scale.Here,we successfully developed the direct photolithography for WOx nanoparticles based on in situ photo-induced ligand exchange.This strategy enabled us to achieve ultra-high resolution efficiently(line width<4μm,the best resolution for reported inorganic electrochromic materials).Additionally,the resulting device exhibited impressive electrochromic performance,such as fast response(<1 s at 0 V),high coloration efficiency(119.5 cm^(2) C^(−1)),good optical modulation(55.9%),and durability(>3600 cycles),as well as promising applications in electronic logos,pixelated displays,flexible electronics,etc.The success and advancements presented here are expected to inspire and accelerate research and development(R&D)in high-resolution non-emissive displays and other ultra-fine micro-electronics.
基金supported by the National Natural Science Foundation of China(Grant No.22479097)the Shanghai Science and Technology Committee(Grant No.23ZR1433000)the National High-Level Talent Program for Young Scholars,the Start-up Fund(F.S.)from Shanghai Jiao Tong University.
文摘Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)accessibility results in a universal self-adaptive structural reconstruction from Cu_(2)O to Cu@CuxO composites,ending with feeding gas-dependent microstructures and catalytic performances.The CO_(2)-rich atmosphere favors reconstruction for CO_(2)RR,whereas the CO_(2)-deficient one prefers that for hydrogen evolution reaction.With the assistance of spectroscopic analysis and theoretical calculations,we uncover a CO_(2)-induced passivation behavior by identifying a reductionresistant but catalytic active Cu(I)-rich amorphous layer stabilized by*CO intermediates.Additionally,we find extra CO production is indispensable for the robust production of C2H4.An inverse correlation between durability and FECO/FEC2H4 is disclosed,suggesting that the selfstabilization process involving the absorption of*CO intermediates on Cu(I)sites is essential for durable electrolysis.Guided by this insight,we design hollow Cu_(2)O nanospheres for durable and selective CO_(2)RR electrolysis in producing C2H4.Our work recognizes the previously overlooked passivation reconstruction and self-stabilizing behavior and highlights the critical role of the local atmosphere in modulating reconstruction and catalytic processes.
基金support from the National Natural Science Foundation of China(62275057)the Guangxi Natural Science Foundation(2023GXNSFFA026004 and 2022GXNSFDA035066)+2 种基金the Innovation Project of Guangxi Graduate Education(YCBZ2024034)Natural Science Foundation of Ningbo under grant(2022J149)Natural Science Foundation of Ningbo under grant(2022A-230-G)
文摘Trap-assisted charge recombination is one of the primary limitationsof restricting the performance of organic solar cells. However, effectivelyreducing the presence of traps in the photoactive layer remains challenging.Herein, wide bandgap polymer donor PTzBI-dF is demonstrated as an effectivemodulator for enhancing the crystallinity of the bulk heterojunction active layerscomposed of D18 derivatives blended with Y6, leading to dense and orderedmolecular packings, and thus, improves photoluminescence quenching properties.As a result, the photovoltaic devices exhibit reduced trap-assisted charge recombinationlosses, achieving an optimized power conversion efficiency of over 19%.Besides the efficiency enhancement, the devices comprised of PTzBI-dF as athird component simultaneously attain decreased current leakage, improved chargecarrier mobilities, and suppressed bimolecular charge recombination, leading toreduced energy losses. The advanced crystalline structures induced by PTzBI-dFand its characteristics, such as well-aligned energy level, and complementaryabsorption spectra, are ascribed to the promising performance improvements.Our findings suggest that donor phase engineering is a feasible approach to tuning the molecular packings in the active layer, providingguidelines for designing effective morphology modulators for high-performance organic solar cells.
基金financial support from the National Key Research and Development Program of China(2021YFB 3501501)the National Natural Science Foundation of China(No.22225803,22038001,22108007 and 22278011)+1 种基金Beijing Natural Science Foundation(No.Z230023)Beijing Science and Technology Commission(No.Z211100004321001).
文摘The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design platform.High-throughput screening of catalytic performance is feasible since the large MOF structure database is available.In this study,we report a machine learning model for high-throughput screening of MOF catalysts for the CO_(2) cycloaddition reaction.The descriptors for model training were judiciously chosen according to the reaction mechanism,which leads to high accuracy up to 97%for the 75%quantile of the training set as the classification criterion.The feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding.12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100℃ and 1 bar within one day using the model,and 239 potentially efficient catalysts were discovered.Among them,MOF-76(Y)achieved the top performance experimentally among reported MOFs,in good agreement with the prediction.
