Myelin,made by oligodendrocytes(OLs)in the central nervous system(CNS),is essential for neural transmission.In particular,myelin facilitates communication across the long connections between different brain regions th...Myelin,made by oligodendrocytes(OLs)in the central nervous system(CNS),is essential for neural transmission.In particular,myelin facilitates communication across the long connections between different brain regions that form the white matter.Myelinated segments also provide metabolic intermediates to axons,supporting their demanding energetic needs.Genetic disorders that disrupt myelin formation result in progressive neurologic degeneration.展开更多
The production of valuable chemicals using copper(Cu)catalysts via electrochemical CO or CO_(2)reduction reactions(CORR and CO_(2)RR)has shown great potential in the field of sustainable energy conversion[1].Previous ...The production of valuable chemicals using copper(Cu)catalysts via electrochemical CO or CO_(2)reduction reactions(CORR and CO_(2)RR)has shown great potential in the field of sustainable energy conversion[1].Previous research has primarily focused on analyzing the behavior of reaction intermediates or solely on the dynamics within the solution phase,while the synergistic effects between surface species and the solution,particularly the interfacial water and its non-covalent interactions with the Cu surface,have remained partially understood[2].展开更多
The development of bifunctional electrocatalysts capable of integrating biomass-derived platform molecule oxidation with organic reduction offers a promising strategy for simultaneously enhancing energy efficiency and...The development of bifunctional electrocatalysts capable of integrating biomass-derived platform molecule oxidation with organic reduction offers a promising strategy for simultaneously enhancing energy efficiency and generating high-value chemicals.However,designing catalysts that exhibit both high activity and stability in integrated systems remains a significant challenge.Herein,we report a selfsupported electrode composed of nitrogen-doped carbonized wood(NCW)supported NiCo nanosheets(NiCo_(0.3)/NCW)that enables the electrocatalytic 5-hydroxymethylfurfural oxidation to produce 2,5-furandicarboxylic acid(FDCA)and the nitrobenzene reduction to yield aniline in an integrated electrochemical cell.The NiCo_(0.3)/NCW electrode achieves the production of FDCA and aniline at a low cell voltage of 1.7 V,with~99%anodic and~92%cathodic Faradaic efficiencies,respectively.Experimental characterizations disclose that the hierarchical porous NCW architecture promotes the dispersion of active sites,while nitrogen doping strengthens metal-support interactions.In-situ spectroscopic experiments combined with density functional theory(DFT)calculations reveal that cobalt incorporation tunes the electronic structure of nickel,thus optimizing substrate and intermediate adsorption,and lowering energy barriers.These effects ultimately enhance the performance of the natural wood-derived catalyst in integrated biomass valorization and selective organic electrosynthesis.展开更多
Inborn errors of metabolism(IEMs)are a large group of disorders resulting from deficient activities in several metabolic pathways due to the dysfunction of a distinct enzyme associated with a biochemical pathway[1,2]....Inborn errors of metabolism(IEMs)are a large group of disorders resulting from deficient activities in several metabolic pathways due to the dysfunction of a distinct enzyme associated with a biochemical pathway[1,2].Toxic intermediates will be produced due to the dysfunction of biochemical pathways.The liver is responsible for many essential metabolic processes,therefore it becomes one of the most severely affected organ by metabolic diseases[3].Early onset of liver disorders in IEMs includes jaundice,hepatomegaly,splenomegaly,ascites,hepatic encephalopathy,and liver failure[4].In infants and young children under 3 years old with acute liver failure(ALF),IEMs account for 18.9%-43%[5].展开更多
Fabrication of large-area perovskite solar modules under ambient air conditions remains a critical challenge due to air sensitivity of perovskite intermediate phases during crystallization.Here,we introduce 2-iodoimid...Fabrication of large-area perovskite solar modules under ambient air conditions remains a critical challenge due to air sensitivity of perovskite intermediate phases during crystallization.Here,we introduce 2-iodoimidazole(IIZ)into the perovskite precursor,enabling the formation of an air-stable pureδ-phase intermediate,which,upon annealing,fully transforms into a highly orientedα-phase perovskite film with reduced defects and variability.Leveraging this approach,we achieve a stabilized power conversion efficiency of 20.9%for 927.5 cm^(2)perovskite solar modules with high reproducibility.The encapsulated modules meet stringent international photovoltaic testing standards(IEC61215:2021),demonstrating excellent stability under continuous operation,thermal cycling(-40 to 85℃)and damp heat(85℃ and 85%relative humidity).展开更多
When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.Howe...When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.However,the key to the efficiency and return on investment of this hybrid energy system lies in the expected lifetime of the SOEC.This study assessed Ni-YSZ|YSZ|GDC|LSC fuel electrode support cells’long-term stability during electrolysis at 650℃with a current density of−0.5Acm^(−2)over 1818 h.The average voltage degradation rate of 2.63%kh^(−1)unfolded in two phases:an initial rapid decay(90 to 1120 h at 3.58%kh^(−1))and a stable decay(1120 to 1818 h at 2.14%kh^(−1)),emphasizing SOECs’probability coupling with nuclear reactors at 650℃.Post-1818-hour electrolysis revealed nickel particle formation associated with Ni(OH)_(x)diffusion and re-deposition,alongside a strontium-containing layer causing interface cracking.Despite minimal strontium segregation in the EDS,XPS data indicated surface segregation of Sr.This study provides crucial insights into prolonged SOEC operation,highlighting both its potential and challenges.展开更多
Ambient-air,moisture-assisted annealing is widely used in fabricating perovskite solar cells(PSCs).However,the inherent sensitivity of perovskite intermediate-phase to moisture—due to fast and spontaneous intermolecu...Ambient-air,moisture-assisted annealing is widely used in fabricating perovskite solar cells(PSCs).However,the inherent sensitivity of perovskite intermediate-phase to moisture—due to fast and spontaneous intermolecular exchange reaction—requires strict control of ambient humidity and immediate thermal annealing treatment,raising manufacturing costs and causing fast nucleation of perovskite films.We report herein a self-buffered molecular migration strategy to slow down the intermolecular exchange reaction by introducing a n-butylammonium bromide shielding layer,which limits moisture diffusion into intermediate-phase film.This further endows the notably wide nucleation time and humidity windows for perovskite crystallization in ambient air.Consequently,the optimized 1.68 e V-bandgap n-i-p structured PSC reaches a record-high reverse-scan(RS)PCE of 22.09%.Furthermore,the versatility and applicability of as-proposed self-buffered molecular migration strategy are certified by employing various shielding materials and 1.53 eV-/1.77 eV-bandgap perovskite materials.The n-i-p structured PSCs based on 1.53 eV-and 1.77 eV-bandgap perovskite films achieve outstanding RS PCEs of 25.23%and 19.09%,respectively,both of which are beyond of the state-of-the-art ambient-air processed PSCs.展开更多
Cation disordering is a common issue in Ni-rich cathodes that significantly degrades cycle life and compromises safety.The cubic rock-salt phase formation and the slow oxidation kinetics of Ni^(2+)during solid-state s...Cation disordering is a common issue in Ni-rich cathodes that significantly degrades cycle life and compromises safety.The cubic rock-salt phase formation and the slow oxidation kinetics of Ni^(2+)during solid-state sintering are widely recognized as the principal causes of these structural defects.To solve this issue,a topotactic soft-chemical precursor engineering strategy is proposed for use in aqueous solution.By utilizing the layered structure of the precursor,this method allows for selective proton extraction and efficient Ni^(2+)oxidation,along with rapid Li+intercalation to form a layered lithiated intermediate.This intermediate crystallizes without further phase transitions during subsequent heat treatment,preventing structural defects caused by complex phase evolution and slow ion diffusion.The resulting cathode exhibits a long-range ordered layered structure and a uniform phase distribution,enabling efficient Li+insertion and extraction.Electrochemical tests reveal a high discharge capacity of 229.6 mAh g^(−1)and an initial coulombic efficiency of 95.77%at 0.1 C,greatly exceeding the performance of a conventionally synthesized cathode(210.3 mAh g^(−1),88.93%).Improved Li^(+)transport kinetics reduces phase-transition hysteresis and alleviates stress concentration,resulting in better cycling stability with a capacity retention of 85.3%after 300 cycles,compared to 61.5%for the conventional sample.This work presents a scalable and effective synthesis route for Ni-rich cathodes with reduced structural disorder and extended lifespan,providing valuable insights into how the regulation of intermediate phases influences electrochemical performance in high-performance Ni-rich cathodes.展开更多
文摘The photochemical[2+2]cycloaddition reaction of carbonyl compunds and alkenes was studied by photochemical induced dynamic nuclear spin polarization.
基金support held by JPA,Collaborative Network Award BRAVEinMS,Grant/Award Number:PA-1604-08492(MG)from the Multiple Sclerosis Society of Canada,Grant/Award Number:1038154(to TEK).
文摘Myelin,made by oligodendrocytes(OLs)in the central nervous system(CNS),is essential for neural transmission.In particular,myelin facilitates communication across the long connections between different brain regions that form the white matter.Myelinated segments also provide metabolic intermediates to axons,supporting their demanding energetic needs.Genetic disorders that disrupt myelin formation result in progressive neurologic degeneration.
文摘The production of valuable chemicals using copper(Cu)catalysts via electrochemical CO or CO_(2)reduction reactions(CORR and CO_(2)RR)has shown great potential in the field of sustainable energy conversion[1].Previous research has primarily focused on analyzing the behavior of reaction intermediates or solely on the dynamics within the solution phase,while the synergistic effects between surface species and the solution,particularly the interfacial water and its non-covalent interactions with the Cu surface,have remained partially understood[2].
基金financially supported by the National Natural Science Foundation of China(22504118,T2293692,22525042 and 22373080)the Natural Science Foundation of Fujian Province of China(2025J08010)+3 种基金the Natural Science Foundation of Xiamen,China(3502Z202471009 and 3502Z202472001)funding support from the Fundamental Research Funds for the Central Universities(20720240054)the Nan-qiang Youth Scholar Program of Xiamen Universitythe Xiaomi Young Talents Program/Xiaomi Foundation。
文摘The development of bifunctional electrocatalysts capable of integrating biomass-derived platform molecule oxidation with organic reduction offers a promising strategy for simultaneously enhancing energy efficiency and generating high-value chemicals.However,designing catalysts that exhibit both high activity and stability in integrated systems remains a significant challenge.Herein,we report a selfsupported electrode composed of nitrogen-doped carbonized wood(NCW)supported NiCo nanosheets(NiCo_(0.3)/NCW)that enables the electrocatalytic 5-hydroxymethylfurfural oxidation to produce 2,5-furandicarboxylic acid(FDCA)and the nitrobenzene reduction to yield aniline in an integrated electrochemical cell.The NiCo_(0.3)/NCW electrode achieves the production of FDCA and aniline at a low cell voltage of 1.7 V,with~99%anodic and~92%cathodic Faradaic efficiencies,respectively.Experimental characterizations disclose that the hierarchical porous NCW architecture promotes the dispersion of active sites,while nitrogen doping strengthens metal-support interactions.In-situ spectroscopic experiments combined with density functional theory(DFT)calculations reveal that cobalt incorporation tunes the electronic structure of nickel,thus optimizing substrate and intermediate adsorption,and lowering energy barriers.These effects ultimately enhance the performance of the natural wood-derived catalyst in integrated biomass valorization and selective organic electrosynthesis.
文摘Inborn errors of metabolism(IEMs)are a large group of disorders resulting from deficient activities in several metabolic pathways due to the dysfunction of a distinct enzyme associated with a biochemical pathway[1,2].Toxic intermediates will be produced due to the dysfunction of biochemical pathways.The liver is responsible for many essential metabolic processes,therefore it becomes one of the most severely affected organ by metabolic diseases[3].Early onset of liver disorders in IEMs includes jaundice,hepatomegaly,splenomegaly,ascites,hepatic encephalopathy,and liver failure[4].In infants and young children under 3 years old with acute liver failure(ALF),IEMs account for 18.9%-43%[5].
基金supported by the National Key R&D Program of China(2023YFB4204504)National Science Fund for Dis-tinguished Young Scholars(T2325016)+7 种基金National Natural Science Foundation of China(U21A2076)Natural Science Foundation of Jiangsu Province(BK20232022,BE2022021 and BE2022026)Fundamental Research Funds for the Central Universities(0213/14380206 and 0205/14380252)Frontiers Science Center for Critical Earth Material Cycling Fund(DLTD2109 and 2024ZD06)Program for Innovative Talents and Entrepreneur in JiangsuChina Postdoctoral Science Foundation(2023M731579)Jiangsu Funding Program for Excellent Postdoctoral Talent(2023ZB348)Postdoctoral Innovative Talents Support Project from the China Postdoctoral Science Foundation(BX20230157)。
文摘Fabrication of large-area perovskite solar modules under ambient air conditions remains a critical challenge due to air sensitivity of perovskite intermediate phases during crystallization.Here,we introduce 2-iodoimidazole(IIZ)into the perovskite precursor,enabling the formation of an air-stable pureδ-phase intermediate,which,upon annealing,fully transforms into a highly orientedα-phase perovskite film with reduced defects and variability.Leveraging this approach,we achieve a stabilized power conversion efficiency of 20.9%for 927.5 cm^(2)perovskite solar modules with high reproducibility.The encapsulated modules meet stringent international photovoltaic testing standards(IEC61215:2021),demonstrating excellent stability under continuous operation,thermal cycling(-40 to 85℃)and damp heat(85℃ and 85%relative humidity).
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA0400000),the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2021253)+1 种基金the Major Science and Technology Projects of China National Offshore Oil Corporation Limited during the 14th Five Year Plan(No.KJGG-2022-12-CCUS-030500)the Photon Science Center for Carbon Neutrality of Chinese Academy of Science.
文摘When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.However,the key to the efficiency and return on investment of this hybrid energy system lies in the expected lifetime of the SOEC.This study assessed Ni-YSZ|YSZ|GDC|LSC fuel electrode support cells’long-term stability during electrolysis at 650℃with a current density of−0.5Acm^(−2)over 1818 h.The average voltage degradation rate of 2.63%kh^(−1)unfolded in two phases:an initial rapid decay(90 to 1120 h at 3.58%kh^(−1))and a stable decay(1120 to 1818 h at 2.14%kh^(−1)),emphasizing SOECs’probability coupling with nuclear reactors at 650℃.Post-1818-hour electrolysis revealed nickel particle formation associated with Ni(OH)_(x)diffusion and re-deposition,alongside a strontium-containing layer causing interface cracking.Despite minimal strontium segregation in the EDS,XPS data indicated surface segregation of Sr.This study provides crucial insights into prolonged SOEC operation,highlighting both its potential and challenges.
基金the financial support from the National Key R&D Program of China(2021YFF0500500)the National Natural Science Foundation of China(62474131,62274132,and 62204189)。
文摘Ambient-air,moisture-assisted annealing is widely used in fabricating perovskite solar cells(PSCs).However,the inherent sensitivity of perovskite intermediate-phase to moisture—due to fast and spontaneous intermolecular exchange reaction—requires strict control of ambient humidity and immediate thermal annealing treatment,raising manufacturing costs and causing fast nucleation of perovskite films.We report herein a self-buffered molecular migration strategy to slow down the intermolecular exchange reaction by introducing a n-butylammonium bromide shielding layer,which limits moisture diffusion into intermediate-phase film.This further endows the notably wide nucleation time and humidity windows for perovskite crystallization in ambient air.Consequently,the optimized 1.68 e V-bandgap n-i-p structured PSC reaches a record-high reverse-scan(RS)PCE of 22.09%.Furthermore,the versatility and applicability of as-proposed self-buffered molecular migration strategy are certified by employing various shielding materials and 1.53 eV-/1.77 eV-bandgap perovskite materials.The n-i-p structured PSCs based on 1.53 eV-and 1.77 eV-bandgap perovskite films achieve outstanding RS PCEs of 25.23%and 19.09%,respectively,both of which are beyond of the state-of-the-art ambient-air processed PSCs.
基金the financial support from the Central South University Fundamental Research Funds (Grant No.2025ZZTS0444)the Innovation-Driven Research Program(Grant No. 2023 CXQD053)+3 种基金the National Natural Science Foundation of China (Grant No. 52274310)the financial support (Project No.H202111040350002)the provision of the hydroxide precursors from Ningbo Ronbay New Energy Technology Co.,Ltdsupported in part by the High-Performance Computing Center of Central South University
文摘Cation disordering is a common issue in Ni-rich cathodes that significantly degrades cycle life and compromises safety.The cubic rock-salt phase formation and the slow oxidation kinetics of Ni^(2+)during solid-state sintering are widely recognized as the principal causes of these structural defects.To solve this issue,a topotactic soft-chemical precursor engineering strategy is proposed for use in aqueous solution.By utilizing the layered structure of the precursor,this method allows for selective proton extraction and efficient Ni^(2+)oxidation,along with rapid Li+intercalation to form a layered lithiated intermediate.This intermediate crystallizes without further phase transitions during subsequent heat treatment,preventing structural defects caused by complex phase evolution and slow ion diffusion.The resulting cathode exhibits a long-range ordered layered structure and a uniform phase distribution,enabling efficient Li+insertion and extraction.Electrochemical tests reveal a high discharge capacity of 229.6 mAh g^(−1)and an initial coulombic efficiency of 95.77%at 0.1 C,greatly exceeding the performance of a conventionally synthesized cathode(210.3 mAh g^(−1),88.93%).Improved Li^(+)transport kinetics reduces phase-transition hysteresis and alleviates stress concentration,resulting in better cycling stability with a capacity retention of 85.3%after 300 cycles,compared to 61.5%for the conventional sample.This work presents a scalable and effective synthesis route for Ni-rich cathodes with reduced structural disorder and extended lifespan,providing valuable insights into how the regulation of intermediate phases influences electrochemical performance in high-performance Ni-rich cathodes.
