铁铬氧化还原液流电池(ICRFB)是一种具有成本效益的可规模化储能系统,其利用资源丰富、低成本的铬和铁作为电解液的活性物质。然而,ICRFB存在Cr^(3+)/Cr^(2+)电化学活性低、负极易产生严重的析氢反应(HER)等问题。本文报道了一种简单的...铁铬氧化还原液流电池(ICRFB)是一种具有成本效益的可规模化储能系统,其利用资源丰富、低成本的铬和铁作为电解液的活性物质。然而,ICRFB存在Cr^(3+)/Cr^(2+)电化学活性低、负极易产生严重的析氢反应(HER)等问题。本文报道了一种简单的合成策略,即通过自聚合和湿化学还原方法结合煅烧处理,在氮掺杂石墨毡(GF)表面沉积了非晶态铋(Bi)纳米颗粒(NPs),其作为ICRFB的负极材料时可展示出高效的电化学性能。生成的BiNPs与H+形成中间体,极大地抑制了HER副反应。此外,Bi的引入和GF表面的N掺杂通过协同作用显著提高了Fe^(2+)/Fe^(3+)和Cr^(3+)/Cr^(2+)的电化学活性,降低了电荷传递电阻,提高了反应传质速率。在不同的电流密度下,经25次循环,库仑效率仍高达97.7%。在60.0 mA cm^(-2)电流密度下,能量效率达到85.8%,超过了许多其他报道的材料。循环100次后容量达到862.7 mAh/L,约为GF的5.3倍。展开更多
Climate change caused by the increasing emission of CO_(2)to the atmosphere has become a global concern.To ameliorate this issue,converting CO_(2)into valuable chemicals is highly desirable,enabling a sustainable low-...Climate change caused by the increasing emission of CO_(2)to the atmosphere has become a global concern.To ameliorate this issue,converting CO_(2)into valuable chemicals is highly desirable,enabling a sustainable low-carbon future.To this end,developing efficient catalytic systems for CO_(2)conversion has sparked intense interests from both academia and industry.Taking advantage of their highly porous structures and unique properties,metal−organic frameworks(MOFs)have shown great potential as heterogeneous catalysts for CO_(2)conversion.Various transformations involving CO_(2)have been accomplished over MOFs-based materials.Here we provide a comprehensive and up-to-date review on recent advances of heterogeneous CO_(2)thermocatalysis using MOFs,highlighting relationships between structures and properties.Special attention is given to the design strategies for improving the catalytic performance of MOFs.Avenues available to enrich the catalytic active sites in MOF structures are stressed and their respective impacts on CO_(2)conversion efficiency are presented.The synergistic effects between each active site within the structure of MOFs and derivatives are discussed.In the end,future perspectives and challenges in CO_(2)conversion by heterogeneous catalysis with MOFs are described.展开更多
文摘铁铬氧化还原液流电池(ICRFB)是一种具有成本效益的可规模化储能系统,其利用资源丰富、低成本的铬和铁作为电解液的活性物质。然而,ICRFB存在Cr^(3+)/Cr^(2+)电化学活性低、负极易产生严重的析氢反应(HER)等问题。本文报道了一种简单的合成策略,即通过自聚合和湿化学还原方法结合煅烧处理,在氮掺杂石墨毡(GF)表面沉积了非晶态铋(Bi)纳米颗粒(NPs),其作为ICRFB的负极材料时可展示出高效的电化学性能。生成的BiNPs与H+形成中间体,极大地抑制了HER副反应。此外,Bi的引入和GF表面的N掺杂通过协同作用显著提高了Fe^(2+)/Fe^(3+)和Cr^(3+)/Cr^(2+)的电化学活性,降低了电荷传递电阻,提高了反应传质速率。在不同的电流密度下,经25次循环,库仑效率仍高达97.7%。在60.0 mA cm^(-2)电流密度下,能量效率达到85.8%,超过了许多其他报道的材料。循环100次后容量达到862.7 mAh/L,约为GF的5.3倍。
文摘Climate change caused by the increasing emission of CO_(2)to the atmosphere has become a global concern.To ameliorate this issue,converting CO_(2)into valuable chemicals is highly desirable,enabling a sustainable low-carbon future.To this end,developing efficient catalytic systems for CO_(2)conversion has sparked intense interests from both academia and industry.Taking advantage of their highly porous structures and unique properties,metal−organic frameworks(MOFs)have shown great potential as heterogeneous catalysts for CO_(2)conversion.Various transformations involving CO_(2)have been accomplished over MOFs-based materials.Here we provide a comprehensive and up-to-date review on recent advances of heterogeneous CO_(2)thermocatalysis using MOFs,highlighting relationships between structures and properties.Special attention is given to the design strategies for improving the catalytic performance of MOFs.Avenues available to enrich the catalytic active sites in MOF structures are stressed and their respective impacts on CO_(2)conversion efficiency are presented.The synergistic effects between each active site within the structure of MOFs and derivatives are discussed.In the end,future perspectives and challenges in CO_(2)conversion by heterogeneous catalysis with MOFs are described.
