The efficiency of the catalytic decomposition of ammonia is a central challenge for the use of ammonia as a potential hydrogen vector and fuel for heavy-duty applications. In this study, we explore the promotional effect of alkali and earth-alkaline metals on cobalt and nickel catalysts for ammonia decomposition in a computational screening. We elucidate the strong influence of the recently proposed spin promotion effect on catalytic activity and identify barium as a promising and stable promoter of Co under the relevant reaction conditions. The predictions are validated experimentally through the study of a BaCo catalyst, ultimately yielding a metal-based hydrogen productivity of 12.2 mol g_Co⁻¹ h⁻¹ at 500 °C, common for state-of-the-art ruthenium catalysts. This work not only reports the successful development of a novel catalyst but also provides validation for the spin-promotion effect and its substantial influence on catalyst performance.

中文翻译：

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钡掺杂钴催化剂的理论指导开发


氨的催化分解效率是将氨用作重型应用的潜在氢载体和燃料的核心挑战。在这项研究中，我们探讨了碱金属和土碱金属对钴和镍催化剂在计算筛选中氨分解的促进作用。我们阐明了最近提出的自旋促进作用对催化活性的强烈影响，并确定钡在相关反应条件下是有前途且稳定的 Co 促进剂。通过对 BaCo 催化剂的研究，这些预测得到了实验验证，最终在 500 °C 下产生了 12.2 mol g ^{Co-1 h-1} 的金属基氢产能，这在最先进的钌催化剂中很常见。这项工作不仅报道了一种新型催化剂的成功开发，还为自旋促进效应及其对催化剂性能的实质性影响提供了验证。