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Atomically Isolated Rh Sites within Highly Branched Rh2Sb Nanostructures Enhance Bifunctional Hydrogen Electrocatalysis
Advanced Materials ( IF 27.4 ) Pub Date : 2021-09-12 , DOI: 10.1002/adma.202105049 Ying Zhang 1 , Gen Li 1 , Zhonglong Zhao 2 , Lili Han 3 , Yonggang Feng 1 , Shangheng Liu 1 , Bingyan Xu 1 , Honggang Liao 1 , Gang Lu 4 , Huolin L Xin 3 , Xiaoqing Huang 1
Advanced Materials ( IF 27.4 ) Pub Date : 2021-09-12 , DOI: 10.1002/adma.202105049 Ying Zhang 1 , Gen Li 1 , Zhonglong Zhao 2 , Lili Han 3 , Yonggang Feng 1 , Shangheng Liu 1 , Bingyan Xu 1 , Honggang Liao 1 , Gang Lu 4 , Huolin L Xin 3 , Xiaoqing Huang 1
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Breaking the bottleneck of hydrogen oxidation/evolution reactions (HOR/HER) in alkaline media is of tremendous importance for the development of anion exchange membrane fuel cells/water electrolyzers. Atomically dispersed active sites are known to exhibit excellent activity and selectivity toward diverse catalytic reactions. Here, a class of unique Rh2Sb nanocrystals with multiple nanobranches (denoted as Rh2Sb NBs) and atomically dispersed Rh sites are reported as promising electrocatalysts for alkaline HOR/HER. Rh2Sb NBs/C exhibits superior HER performance with a low overpotential and a small Tafel slope, outperforming both Rh NBs/C and commercial Pt/C. Significantly, Rh2Sb NBs show outstanding HOR performance of which the HOR specific activity and mass activity are about 9.9 and 10.1 times to those of Rh NBs/C, and about 4.2 and 3.7 times to those of Pt/C, respectively. Strikingly, Rh2Sb NBs can also exhibit excellent CO tolerance during HOR, whose activity can be largely maintained even at 100 ppm CO impurity. Density functional theory calculations reveal that the unsaturated Rh sites on Rh2Sb NBs surface are crucial for the enhanced alkaline HER and HOR activities. This work provides a unique catalyst design for efficient hydrogen electrocatalysis, which is critical for the development of alkaline fuel cells and beyond.
中文翻译：
高度支化的 Rh2Sb 纳米结构中原子分离的 Rh 位点增强双功能氢电催化
打破碱性介质中氢氧化/析出反应（HOR/HER）的瓶颈对于阴离子交换膜燃料电池/水电解槽的发展具有极其重要的意义。已知原子分散的活性位点对各种催化反应表现出优异的活性和选择性。在这里，一类具有多个纳米分支（表示为 Rh 2 Sb NBs）和原子分散的 Rh 位点的独特 Rh 2 Sb 纳米晶体被报道为有前途的碱性 HOR/HER 电催化剂。Rh 2 Sb NBs/C 表现出优异的 HER 性能，具有低过电位和小塔菲尔斜率，优于 Rh NBs/C 和商业 Pt/C。值得注意的是，Rh 2Sb NBs表现出优异的HOR性能，其HOR比活度和质量活度分别是Rh NBs/C的9.9和10.1倍，Pt/C的4.2和3.7倍。引人注目的是，Rh 2 Sb NBs 还可以表现出出色的 CO 耐受性期间 HOR，其活动可以在很大程度上保持即使在 100 ppm CO 杂质。密度泛函理论计算表明，Rh 2 Sb NBs 表面上的不饱和 Rh 位点对于增强碱性 HER 和 HOR 活性至关重要。这项工作为高效的氢电催化提供了独特的催化剂设计，这对于碱性燃料电池及其他方面的发展至关重要。
更新日期：2021-10-27
中文翻译：
高度支化的 Rh2Sb 纳米结构中原子分离的 Rh 位点增强双功能氢电催化
打破碱性介质中氢氧化/析出反应（HOR/HER）的瓶颈对于阴离子交换膜燃料电池/水电解槽的发展具有极其重要的意义。已知原子分散的活性位点对各种催化反应表现出优异的活性和选择性。在这里，一类具有多个纳米分支（表示为 Rh 2 Sb NBs）和原子分散的 Rh 位点的独特 Rh 2 Sb 纳米晶体被报道为有前途的碱性 HOR/HER 电催化剂。Rh 2 Sb NBs/C 表现出优异的 HER 性能，具有低过电位和小塔菲尔斜率，优于 Rh NBs/C 和商业 Pt/C。值得注意的是，Rh 2Sb NBs表现出优异的HOR性能，其HOR比活度和质量活度分别是Rh NBs/C的9.9和10.1倍，Pt/C的4.2和3.7倍。引人注目的是，Rh 2 Sb NBs 还可以表现出出色的 CO 耐受性期间 HOR，其活动可以在很大程度上保持即使在 100 ppm CO 杂质。密度泛函理论计算表明，Rh 2 Sb NBs 表面上的不饱和 Rh 位点对于增强碱性 HER 和 HOR 活性至关重要。这项工作为高效的氢电催化提供了独特的催化剂设计，这对于碱性燃料电池及其他方面的发展至关重要。
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