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Improved Catalyst Performance for the Oxygen Evolution Reaction under a Chiral Bias
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-11-10 , DOI: 10.1021/acscatal.4c04477 Aravind Vadakkayil, Wiley A. Dunlap-Shohl, Meera Joy, Brian P. Bloom, David H. Waldeck
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-11-10 , DOI: 10.1021/acscatal.4c04477 Aravind Vadakkayil, Wiley A. Dunlap-Shohl, Meera Joy, Brian P. Bloom, David H. Waldeck
The oxygen evolution reaction (OER) remains an important bottleneck for widespread implementation of a hydrogen economy. While improvements in the OER can be realized by spin polarizing the reaction intermediates, these methods often rely on applying external magnetic fields to ferromagnetic catalysts or by adsorbing chiral molecules onto the catalyst. Here, we show that the addition of chiral additives to the conductive binder supporting the catalysts enhances the selectivity for O2 formation and results in exceedingly high mass activities. The results are explained within the context of a statistical model in which the additives are hypothesized to act as a localized chiral bias that enhances radical intermediate coupling. More broadly, these studies illustrate a flexible design motif for improving OER catalysis that persists under different pH conditions, is independent of the choice of catalyst, and can be extrapolated to other chemical reactions.
中文翻译:
提高手性偏压下析氧反应的催化剂性能
析氧反应 (OER) 仍然是广泛实施氢经济的重要瓶颈。虽然可以通过自旋极化反应中间体来实现 OER 的改进,但这些方法通常依赖于对铁磁催化剂施加外部磁场或将手性分子吸附到催化剂上。在这里,我们表明,在支持催化剂的导电粘合剂中添加手性添加剂可以提高 O2 形成的选择性,并导致极高的质量活性。在统计模型的背景下对结果进行了解释,其中假设添加剂充当增强自由基中间偶联的局部手性偏倚。更广泛地说,这些研究说明了一种用于改进 OER 催化的灵活设计基序,该基序在不同的 pH 条件下持续存在,与催化剂的选择无关,并且可以外推到其他化学反应。
更新日期:2024-11-12
中文翻译:
提高手性偏压下析氧反应的催化剂性能
析氧反应 (OER) 仍然是广泛实施氢经济的重要瓶颈。虽然可以通过自旋极化反应中间体来实现 OER 的改进,但这些方法通常依赖于对铁磁催化剂施加外部磁场或将手性分子吸附到催化剂上。在这里,我们表明,在支持催化剂的导电粘合剂中添加手性添加剂可以提高 O2 形成的选择性,并导致极高的质量活性。在统计模型的背景下对结果进行了解释,其中假设添加剂充当增强自由基中间偶联的局部手性偏倚。更广泛地说,这些研究说明了一种用于改进 OER 催化的灵活设计基序,该基序在不同的 pH 条件下持续存在,与催化剂的选择无关,并且可以外推到其他化学反应。