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Potassium ions promote electrochemical nitrogen reduction on nano-Au catalysts triggered by bifunctional boron supramolecular assembly
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-06-15 , DOI: 10.1039/d0ta04580b Xue Zhao 1, 2, 3, 4 , Ziqiong Yang 1, 2, 3, 4 , Artem V. Kuklin 5, 6, 7, 8, 9 , Glib V. Baryshnikov 5, 6, 7, 8, 9 , Hans Ågren 5, 6, 7, 8, 9 , Wenjing Wang 4, 10, 11, 12, 13 , Xiaohai Zhou 1, 2, 3, 4, 14 , Haibo Zhang 1, 2, 3, 4, 15
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-06-15 , DOI: 10.1039/d0ta04580b Xue Zhao 1, 2, 3, 4 , Ziqiong Yang 1, 2, 3, 4 , Artem V. Kuklin 5, 6, 7, 8, 9 , Glib V. Baryshnikov 5, 6, 7, 8, 9 , Hans Ågren 5, 6, 7, 8, 9 , Wenjing Wang 4, 10, 11, 12, 13 , Xiaohai Zhou 1, 2, 3, 4, 14 , Haibo Zhang 1, 2, 3, 4, 15
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The electrochemical way of reducing nitrogen to ammonia presents green and economic advantages to dial down irreversible damage caused by the energy-intensive Haber–Bosch process. Here, we introduce an advanced catalyst CB[7]–K2[B12H12]@Au with highly dispersed and ultrafine nano-gold. The CB[7]–K2[B12H12]@Au electrochemically driven ammonia yield and Faraday efficiency is as high as 41.69 μg h−1 mgcat.−1 and 29.53% (at −0.4 V vs. RHE), respectively, reaching the US Department of Energy (DOE) utility index of ambient ammonia production along with excellent cycle stability and tolerance that indicates a high potential of industrial practical value. Experimental results and theoretical calculations show that the key to an excellent electrochemical nitrogen reduction performance lies in the smart design of the CB[7]–K2[B12H12]@Au catalyst combining the stable substrate anchored Au nanoparticles and K+ ions that effectively prevent the hydrogen evolution reaction and polarize *N2 leading to lowering of the rate determining step. This research will promote the further development of electrochemical ammonia production with low environmental impact.
中文翻译：
钾离子促进双功能硼超分子组装引发的纳米金催化剂上的电化学氮还原
将氮还原为氨的电化学方法具有绿色和经济优势，可以减少由耗能的Haber-Bosch工艺造成的不可逆损害。在这里，我们介绍一种具有高度分散和超细纳米金的高级催化剂CB [7] -K 2 [B 12 H 12 ] @Au。CB [7] –K 2 [B 12 H 12 ] @Au电化学驱动的氨收率和法拉第效率高达41.69μgh -1 mg cat。-1和29.53％（在-0.4 V与RHE）分别达到美国能源部（DOE）的环境氨生产效用指数，以及出色的循环稳定性和耐受性，这表明其具有很高的工业实用价值。实验结果和理论计算表明，电化学还原氮性能优异的关键在于CB [7] –K 2 [B 12 H 12 ] @Au催化剂的智能设计，该催化剂结合了稳定的基质锚定的Au纳米粒子和K +离子有效防止氢逸出反应并使* N 2极化导致降低速率确定步骤。这项研究将促进对环境影响较小的电化学氨生产的进一步发展。
更新日期：2020-07-07
中文翻译：
钾离子促进双功能硼超分子组装引发的纳米金催化剂上的电化学氮还原
将氮还原为氨的电化学方法具有绿色和经济优势，可以减少由耗能的Haber-Bosch工艺造成的不可逆损害。在这里，我们介绍一种具有高度分散和超细纳米金的高级催化剂CB [7] -K 2 [B 12 H 12 ] @Au。CB [7] –K 2 [B 12 H 12 ] @Au电化学驱动的氨收率和法拉第效率高达41.69μgh -1 mg cat。-1和29.53％（在-0.4 V与RHE）分别达到美国能源部（DOE）的环境氨生产效用指数，以及出色的循环稳定性和耐受性，这表明其具有很高的工业实用价值。实验结果和理论计算表明，电化学还原氮性能优异的关键在于CB [7] –K 2 [B 12 H 12 ] @Au催化剂的智能设计，该催化剂结合了稳定的基质锚定的Au纳米粒子和K +离子有效防止氢逸出反应并使* N 2极化导致降低速率确定步骤。这项研究将促进对环境影响较小的电化学氨生产的进一步发展。
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