Dear Editor,Psoriasis,a chronic inflammatory cutaneous condition,is characterized by the development of red plaques with silvery scales,significantly affecting patients'quality of life and mental health[1].This co...Dear Editor,Psoriasis,a chronic inflammatory cutaneous condition,is characterized by the development of red plaques with silvery scales,significantly affecting patients'quality of life and mental health[1].This condition is thought to affect approximately 2%of the Western population,with diagnosis peaking in early adulthood[2].Vitamin D,a fat-soluble vitamin,is essential for phospho-calcium metabolism,calcium homeostasis,and bone health.展开更多
Electrocatalytic water splitting for green hydrogen is hindered by the slow oxygen evolution reaction(OER).Replacing OER with ethylene glycol oxidation(EGOR)offers an energy-saving route,coproducing valuable chemicals...Electrocatalytic water splitting for green hydrogen is hindered by the slow oxygen evolution reaction(OER).Replacing OER with ethylene glycol oxidation(EGOR)offers an energy-saving route,coproducing valuable chemicals,but requires efficient,stable,and low-cost catalysts.Here,we report a sulfate-doped NiOOH-Ni(OH)_(2)catalyst(denoted S-NiOOH-Ni(OH)_(2)).SO_(4)^(2-)doping significantly boosts intrinsic activity,enabling exceptional EGOR performance(only 1.45 V for~650 mA cm^(-2)).In situ studies reveal that a unique"structural locking"effect stabilizes the highly activeβ-NiOOH phase within the composite,differing from conventional reconstruction.Notably,we successfully scaled up this catalyst to an industrial-scale electrolyzer(anode area:1386 cm^(2))and constructed an integrated electrochemical-conventional chemical coupling system,which stably produced 290 L of hydrogen and kilogram-scale high-purity potassium diformate(KDF)per batch.Techno-economic analysis confirms strong commercial viability,projecting$7.1 million annual profit and a payback period under one year.This work bridges advanced catalyst design to industrial biomass valorization coupled with hydrogen production.展开更多
Self-supported nanoarrays have emerged as a promising alternative electrocatalyst for alkaline H_(2)O splitting,owing to their accessible active sites and strongly coupled interfaces with current collectors for improv...Self-supported nanoarrays have emerged as a promising alternative electrocatalyst for alkaline H_(2)O splitting,owing to their accessible active sites and strongly coupled interfaces with current collectors for improved mass transfer and stability.Herein,self-supported crystalline/amorphous NiO/Ni(OH)_(2)nanosheet arrays on nickel foam(NF)are fabricated via an in-situ dissolution-deposition hydrothermal growing of Ni(OH)_(2)nanosheets without additional metal sources assisted by a common Lewis base,EDTA,followed by a rapid calcination at 300℃in air.The as-prepared EDTA-NF-12 h exhibits high OER and HER performance under alkaline conditions,requiring 235 mV and 158 mV,respectively,to reach 10 mA cm^(-2),and the decent performance can be maintained for 24 h without obvious degradation.The dual interfaces,i.e.,the dense crystalline/amorphous interfaces within the NiO/Ni(OH)_(2)nanosheet arrays,as well as the intimate interfaces between nanoarrays and NF,both serve as reaction active sites,facilitate electron transfer,and endow the catalyst with high activity and stability.Furthermore,by applying EDTA-Ni^(2+)and other Lewis bases with varying basicities instead of EDTA,the interfaces with the NF substrate are found to promote the formation of crystalline/amorphous interfaces within the nanosheets.This study offers appealing opportunities for tailoring the electrocatalytic performance of self-supported electrodes via dual interface engineering.展开更多
The large volume expansion and rapid capacity attenuation of tin-based electrodes are the main factors limiting their commercial application.The reasonable design of electrode material structure is particularly import...The large volume expansion and rapid capacity attenuation of tin-based electrodes are the main factors limiting their commercial application.The reasonable design of electrode material structure is particularly important for improving its electrochemical performance.Herein,phosphorus-modified graphene encapsulated Sn_(6)O_(4)(OH)_(4)nanoparticles composite(P-Sn_(6)O_(4)(OH)_(4)@RGO)with crystalline-amorphous heterostructure has been successfully designed and prepared.The design of crystalline-amorphous structure has largely enhanced the active sites,and the construction of a graphene encapsulation structure has greatly alleviated volume expansion.Notably,P-Sn_(6)O_(4)(OH)_(4)@RGO obtained an excellent high-rate longterm cycling performance for lithium-ion batteries anode,reaching a high specific capacity of 970 m Ah/g at 1.0 A/g after 1450 cycles.This work demonstrates that restructuring the electrode material's structure and phase through phosphorus modification can effectively improve the electrochemical performance of tin-based electrode materials.展开更多
Developing advanced electrocatalysts to convert CO_(2) into liquid fuels such as C_(2)H_(5)OH is critical for utilizing intermittent renewable energy.The formation of C_(2)H_(5)OH,however,is generally less favored com...Developing advanced electrocatalysts to convert CO_(2) into liquid fuels such as C_(2)H_(5)OH is critical for utilizing intermittent renewable energy.The formation of C_(2)H_(5)OH,however,is generally less favored compared with the other hydrocarbon products from Cu-based electrocatalysts.In this work,an alkanethiolmodified Cu_(2)O nanowire array(OTT-Cu_(2)O) was constructed with asymmetric Cu sites consisting of paired Cu-O and Cu-S motifs to overcome previous limitations of C_(2)H_(5)OH electrosynthesis via CO_(2)RR pathway.This catalyst achieves a high Faradaic efficiency of 45 % for CO_(2)-to-C_(2)H_(5)OH conversion at 300 m A/cm^(2),representing a more than two-fold enhancement over the Cu_(2)O electrode.Mechanistic investigations reveal that the Cu-S site exhibits distinct C-binding capability that stabilizes key intermediates(^(*)OCH_(2) and ^(*)CO),in contrast to the O-affinitive Cu-O site.The asymmetric S-Cu-O configuration promotes thermodynamically favorable asymmetric C-C coupling between ^(*)CO and ^(*)OCH_(2),forming the critical CO-OCH_(2) intermediate and facilitating C_(2)H_(5)OH production,as opposed to symmetric O-Cu-O sites that mainly generate HCOOH.This work offers an effective strategy for designing multi-active-site catalysts toward highly selective CO_(2) reduction to C_(2)H_(5)OH and provides fundamental insight into the reaction mechanism.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.82573974 and 82373475)to Z.Y.
文摘Dear Editor,Psoriasis,a chronic inflammatory cutaneous condition,is characterized by the development of red plaques with silvery scales,significantly affecting patients'quality of life and mental health[1].This condition is thought to affect approximately 2%of the Western population,with diagnosis peaking in early adulthood[2].Vitamin D,a fat-soluble vitamin,is essential for phospho-calcium metabolism,calcium homeostasis,and bone health.
基金the funding from the National Natural Science Foundation of China(22275001)the Project of Anhui Provincial Department of Education(2022AH010004,KJ2021ZD0002)。
文摘Electrocatalytic water splitting for green hydrogen is hindered by the slow oxygen evolution reaction(OER).Replacing OER with ethylene glycol oxidation(EGOR)offers an energy-saving route,coproducing valuable chemicals,but requires efficient,stable,and low-cost catalysts.Here,we report a sulfate-doped NiOOH-Ni(OH)_(2)catalyst(denoted S-NiOOH-Ni(OH)_(2)).SO_(4)^(2-)doping significantly boosts intrinsic activity,enabling exceptional EGOR performance(only 1.45 V for~650 mA cm^(-2)).In situ studies reveal that a unique"structural locking"effect stabilizes the highly activeβ-NiOOH phase within the composite,differing from conventional reconstruction.Notably,we successfully scaled up this catalyst to an industrial-scale electrolyzer(anode area:1386 cm^(2))and constructed an integrated electrochemical-conventional chemical coupling system,which stably produced 290 L of hydrogen and kilogram-scale high-purity potassium diformate(KDF)per batch.Techno-economic analysis confirms strong commercial viability,projecting$7.1 million annual profit and a payback period under one year.This work bridges advanced catalyst design to industrial biomass valorization coupled with hydrogen production.
基金the foundation of Guangdong Engineering Technology Research Center for Hydrogen Energy and Fuel Cells,the Guangdong Provincial Department of Education Innovation Project(No.2022KQNCX056)the Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515110354 and 2021A1515110582)。
文摘Self-supported nanoarrays have emerged as a promising alternative electrocatalyst for alkaline H_(2)O splitting,owing to their accessible active sites and strongly coupled interfaces with current collectors for improved mass transfer and stability.Herein,self-supported crystalline/amorphous NiO/Ni(OH)_(2)nanosheet arrays on nickel foam(NF)are fabricated via an in-situ dissolution-deposition hydrothermal growing of Ni(OH)_(2)nanosheets without additional metal sources assisted by a common Lewis base,EDTA,followed by a rapid calcination at 300℃in air.The as-prepared EDTA-NF-12 h exhibits high OER and HER performance under alkaline conditions,requiring 235 mV and 158 mV,respectively,to reach 10 mA cm^(-2),and the decent performance can be maintained for 24 h without obvious degradation.The dual interfaces,i.e.,the dense crystalline/amorphous interfaces within the NiO/Ni(OH)_(2)nanosheet arrays,as well as the intimate interfaces between nanoarrays and NF,both serve as reaction active sites,facilitate electron transfer,and endow the catalyst with high activity and stability.Furthermore,by applying EDTA-Ni^(2+)and other Lewis bases with varying basicities instead of EDTA,the interfaces with the NF substrate are found to promote the formation of crystalline/amorphous interfaces within the nanosheets.This study offers appealing opportunities for tailoring the electrocatalytic performance of self-supported electrodes via dual interface engineering.
基金supported by the Natural Science Foundation of Shandong Province(Nos.ZR2024QE450,ZR2024QB302 and ZR2024QB004)the Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202211249)Research Program of Qilu Institute of Technology(Nos.QIT 23TP019,QIT23TP010 and QIT24NN007)。
文摘The large volume expansion and rapid capacity attenuation of tin-based electrodes are the main factors limiting their commercial application.The reasonable design of electrode material structure is particularly important for improving its electrochemical performance.Herein,phosphorus-modified graphene encapsulated Sn_(6)O_(4)(OH)_(4)nanoparticles composite(P-Sn_(6)O_(4)(OH)_(4)@RGO)with crystalline-amorphous heterostructure has been successfully designed and prepared.The design of crystalline-amorphous structure has largely enhanced the active sites,and the construction of a graphene encapsulation structure has greatly alleviated volume expansion.Notably,P-Sn_(6)O_(4)(OH)_(4)@RGO obtained an excellent high-rate longterm cycling performance for lithium-ion batteries anode,reaching a high specific capacity of 970 m Ah/g at 1.0 A/g after 1450 cycles.This work demonstrates that restructuring the electrode material's structure and phase through phosphorus modification can effectively improve the electrochemical performance of tin-based electrode materials.
基金financial supports of the National Natural Science Foundation of China (NSFC,Nos.52394202,52476056,and 52301232)the Natural Science Foundation of Chongqing Province (No.2024NSCQ-MSX1109)。
文摘Developing advanced electrocatalysts to convert CO_(2) into liquid fuels such as C_(2)H_(5)OH is critical for utilizing intermittent renewable energy.The formation of C_(2)H_(5)OH,however,is generally less favored compared with the other hydrocarbon products from Cu-based electrocatalysts.In this work,an alkanethiolmodified Cu_(2)O nanowire array(OTT-Cu_(2)O) was constructed with asymmetric Cu sites consisting of paired Cu-O and Cu-S motifs to overcome previous limitations of C_(2)H_(5)OH electrosynthesis via CO_(2)RR pathway.This catalyst achieves a high Faradaic efficiency of 45 % for CO_(2)-to-C_(2)H_(5)OH conversion at 300 m A/cm^(2),representing a more than two-fold enhancement over the Cu_(2)O electrode.Mechanistic investigations reveal that the Cu-S site exhibits distinct C-binding capability that stabilizes key intermediates(^(*)OCH_(2) and ^(*)CO),in contrast to the O-affinitive Cu-O site.The asymmetric S-Cu-O configuration promotes thermodynamically favorable asymmetric C-C coupling between ^(*)CO and ^(*)OCH_(2),forming the critical CO-OCH_(2) intermediate and facilitating C_(2)H_(5)OH production,as opposed to symmetric O-Cu-O sites that mainly generate HCOOH.This work offers an effective strategy for designing multi-active-site catalysts toward highly selective CO_(2) reduction to C_(2)H_(5)OH and provides fundamental insight into the reaction mechanism.
