为了缓解氧化铁光阳极内部和表面的电荷复合,本文引入了一种界面电荷调控策略,利用界面内建电场(IEF)促进电荷的空间分离.水热生长的钛掺杂氧化铁(Hem)纳米棒通过简单的两步浸渍涂层过程,以石墨相氮化碳(g-C_(3)N_(4))和小的三氧化钼(Mo...为了缓解氧化铁光阳极内部和表面的电荷复合,本文引入了一种界面电荷调控策略,利用界面内建电场(IEF)促进电荷的空间分离.水热生长的钛掺杂氧化铁(Hem)纳米棒通过简单的两步浸渍涂层过程,以石墨相氮化碳(g-C_(3)N_(4))和小的三氧化钼(MoO_(3))团簇进行修饰.与原始的Hem相比,得到的Hem/C_(3)N_(4)/MoO_(3)表现出显著增强的光电化学分解水性能,相对于可逆氢电极,在1.23 V时,光阳极电流密度从0.3 mA cm^(-2)显著提高到1.6 mA cm^(-2),入射光子-电流转换效率在300 nm时达到18.4%.结果表明,在Hem/C_(3)N_(4)/MoO_(3)异质结中引入IEF是通过调控界面电荷特性实现的,此界面电荷特性是由Hem/C_(3)N_(4)界面的TypeⅡ能带排列和光阳极表面增强的能带弯曲所引起的,IEF能显著促进电荷的空间分离.研究这一界面电荷调控过程能为基于氧化铁的光阳极和其他半导体器件提供一种简单有效的策略,通过缓解载流子传输动力学的瓶颈,促进电荷的空间分离,实现高效的太阳能转换.展开更多
Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods gr...Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods grown in an aqueous solution, which triggered encouraging improvement in PEC performances.In comparison to the solution-grown pristine a-Fe2 O3 nanorod photoanode that is PEC inefficient and always needs high temperature(>600 °C) activation, the surface sulfurized a-Fe2 O3 nanorods show photocurrent density increased by orders of magnitude, reaching 0.46 mA cmà2 at 1.23 V vs. RHE(reversible hydrogen electrode) under simulated solar illumination. This improvement in PEC performances should be attributed to the synergy of the increased carrier density, the reduced surface charge carrier recombination and the accelerated water oxidation kinetics at the a-Fe2 O3/electrolyte interface, as induced by the incorporation of S ions and the formation of multi-state S species(Fe-Sx-Oy) at the surface of a-Fe2 O3 nanorods. This study paves a new and facile approach to activate a-Fe2 O3 and even other metal oxides as photoelectrodes for improved PEC water splitting performances, by engineering the surface structure to relieve the bottlenecks of charge transfer dynamics and redox reaction kinetics at the electrode/electrolyte interface.展开更多
Vitamin B(VB1),including thiamin,thiamin monophosphate(TMP),and thiamin pyrophosphate(TPP),is an essential micronutrient for all living organisms.Nevertheless,the precise function of VB1 in rice remains unclear.Here,w...Vitamin B(VB1),including thiamin,thiamin monophosphate(TMP),and thiamin pyrophosphate(TPP),is an essential micronutrient for all living organisms.Nevertheless,the precise function of VB1 in rice remains unclear.Here,we described a VB1 auxotrophic mutant,chlorotic lethal seedling(cles)from the mutation of OsTH1,which displayed collapsed chloroplast membrane system and decreased pigment content.OsTH1 encoded a phosphomethylpyrimidine kinase/thiamin-phosphate pyrophosphorylase,and was expressed in various tissues,especially in seedlings,leaves,and young panicles.The VB1 content in cles was markedly reduced,despite an increase in the expression of VB1 synthesis genes.The decreased TPP content affected the tricarboxylic acid cycle,pentose phosphate pathway,and de novo fatty acid synthesis,leading to a reduction in fatty acids(C16:0 and C18:0)and sugars(sucrose and glucose)of cles.Additionally,irregular expression of chloroplast membrane synthesis genes led to membrane collapse.We also found that alternative splicing and translation allowed OsTH1 to be localized to both chloroplast and cytosol.Our study revealed that OsTH1 was an essential enzyme in VB1 biosynthesis and played crucial roles in seedling growth and development by participating in fatty acid and sugar metabolism,providing new perspectives on VB1 function in rice.展开更多
基金supported by the National Key Research and Development Program of China(2018YFB1502003)the National Natural Science Foundation of China(21875183)+2 种基金the Natural Science Basic Research Program of Shaanxi Province(2019JCW-10)the“Fundamental Research Funds for the Central Universities”“The Youth Innovation Team of Shaanxi Universities”。
文摘为了缓解氧化铁光阳极内部和表面的电荷复合,本文引入了一种界面电荷调控策略,利用界面内建电场(IEF)促进电荷的空间分离.水热生长的钛掺杂氧化铁(Hem)纳米棒通过简单的两步浸渍涂层过程,以石墨相氮化碳(g-C_(3)N_(4))和小的三氧化钼(MoO_(3))团簇进行修饰.与原始的Hem相比,得到的Hem/C_(3)N_(4)/MoO_(3)表现出显著增强的光电化学分解水性能,相对于可逆氢电极,在1.23 V时,光阳极电流密度从0.3 mA cm^(-2)显著提高到1.6 mA cm^(-2),入射光子-电流转换效率在300 nm时达到18.4%.结果表明,在Hem/C_(3)N_(4)/MoO_(3)异质结中引入IEF是通过调控界面电荷特性实现的,此界面电荷特性是由Hem/C_(3)N_(4)界面的TypeⅡ能带排列和光阳极表面增强的能带弯曲所引起的,IEF能显著促进电荷的空间分离.研究这一界面电荷调控过程能为基于氧化铁的光阳极和其他半导体器件提供一种简单有效的策略,通过缓解载流子传输动力学的瓶颈,促进电荷的空间分离,实现高效的太阳能转换.
基金financially supported by the National Natural Science Foundation of China (21875183, 51672210 and 51888103)the National Program for Support of Top-notch Young Professionalsthe ‘‘Fundamental Research Funds for the Central Universities”
文摘Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods grown in an aqueous solution, which triggered encouraging improvement in PEC performances.In comparison to the solution-grown pristine a-Fe2 O3 nanorod photoanode that is PEC inefficient and always needs high temperature(>600 °C) activation, the surface sulfurized a-Fe2 O3 nanorods show photocurrent density increased by orders of magnitude, reaching 0.46 mA cmà2 at 1.23 V vs. RHE(reversible hydrogen electrode) under simulated solar illumination. This improvement in PEC performances should be attributed to the synergy of the increased carrier density, the reduced surface charge carrier recombination and the accelerated water oxidation kinetics at the a-Fe2 O3/electrolyte interface, as induced by the incorporation of S ions and the formation of multi-state S species(Fe-Sx-Oy) at the surface of a-Fe2 O3 nanorods. This study paves a new and facile approach to activate a-Fe2 O3 and even other metal oxides as photoelectrodes for improved PEC water splitting performances, by engineering the surface structure to relieve the bottlenecks of charge transfer dynamics and redox reaction kinetics at the electrode/electrolyte interface.
基金supported by the National Natural Science Foundation of China(32170337,31870303)。
文摘Vitamin B(VB1),including thiamin,thiamin monophosphate(TMP),and thiamin pyrophosphate(TPP),is an essential micronutrient for all living organisms.Nevertheless,the precise function of VB1 in rice remains unclear.Here,we described a VB1 auxotrophic mutant,chlorotic lethal seedling(cles)from the mutation of OsTH1,which displayed collapsed chloroplast membrane system and decreased pigment content.OsTH1 encoded a phosphomethylpyrimidine kinase/thiamin-phosphate pyrophosphorylase,and was expressed in various tissues,especially in seedlings,leaves,and young panicles.The VB1 content in cles was markedly reduced,despite an increase in the expression of VB1 synthesis genes.The decreased TPP content affected the tricarboxylic acid cycle,pentose phosphate pathway,and de novo fatty acid synthesis,leading to a reduction in fatty acids(C16:0 and C18:0)and sugars(sucrose and glucose)of cles.Additionally,irregular expression of chloroplast membrane synthesis genes led to membrane collapse.We also found that alternative splicing and translation allowed OsTH1 to be localized to both chloroplast and cytosol.Our study revealed that OsTH1 was an essential enzyme in VB1 biosynthesis and played crucial roles in seedling growth and development by participating in fatty acid and sugar metabolism,providing new perspectives on VB1 function in rice.
