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Regulating the interfacial water structure by tensile strain to boost electrochemical semi-hydrogenation of alkynes
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-05-31 , DOI: 10.1039/d2qi00767c Xudong Xu 1 , Jun Ma 2, 3 , Fangfang Wu 4 , Kaili Zhu 1 , Haiqiao Zhou 1 , Ye Zhang 1 , Xiaoyu Li 1 , Yuhu Zhou 1 , Gan Jia 1 , Dong Liu 2, 3 , Peng Gao 1 , Wei Ye 1
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-05-31 , DOI: 10.1039/d2qi00767c Xudong Xu 1 , Jun Ma 2, 3 , Fangfang Wu 4 , Kaili Zhu 1 , Haiqiao Zhou 1 , Ye Zhang 1 , Xiaoyu Li 1 , Yuhu Zhou 1 , Gan Jia 1 , Dong Liu 2, 3 , Peng Gao 1 , Wei Ye 1
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Electrochemical semi-hydrogenation (ECSH) of alkynes to produce alkenes is an ideal alternative to traditional thermal semi-hydrogenation (TSH) and yet is limited by low conversion yield and product selectivity. Here, we report a new strategy to tune the activity and selectivity of ECSH by regulating the interfacial water structure. The obtained PdCu icosahedrons deliver a greatly enhanced conversion rate and 98.5% alkene selectivity at 96.5% conversion, as well as sustaining about 100 h continuous test. Tensile strain originating from an icosahedral twinned structure is proved to facilitate the formation of an interfacial water structure, especially K+ ion hydrated water (K·H2O) and 2-coordinated hydrogen-bonded water (2-HB·H2O). We also decode the mysterious role of an interfacial water structure in ECSH performance, in which K·H2O speeds up water splitting to produce Hads which in turn accelerates ECSH conversion, and 2-HB·H2O improves alkene selectivity. The findings provide insights into the tuning of the interfacial water structure in electrocatalyst design in proton-coupled hydrogenation from the viewpoint of lattice strain.
中文翻译：
通过拉伸应变调节界面水结构以促进炔烃的电化学半氢化
炔烃的电化学半氢化 (ECSH) 生产烯烃是传统热半氢化 (TSH) 的理想替代方案，但受限于低转化率和产物选择性。在这里，我们报告了一种通过调节界面水结构来调节 ECSH 活性和选择性的新策略。所获得的 PdCu 二十面体在 96.5% 的转化率下提供了显着提高的转化率和 98.5% 的烯烃选择性，并能维持约 100 小时的连续测试。证明源自二十面体孪晶结构的拉伸应变有助于形成界面水结构，特别是K +离子水合水（K·H 2 O）和2-配位氢键水（2-HB·H 2○）。我们还解读了界面水结构在 ECSH 性能中的神秘作用，其中 K·H 2 O 加速水分解产生 H广告，进而加速 ECSH 转化，而 2-HB·H 2 O 提高了烯烃的选择性。这些发现从晶格应变的角度为质子耦合氢化电催化剂设计中界面水结构的调整提供了见解。
更新日期：2022-05-31
中文翻译：
通过拉伸应变调节界面水结构以促进炔烃的电化学半氢化
炔烃的电化学半氢化 (ECSH) 生产烯烃是传统热半氢化 (TSH) 的理想替代方案，但受限于低转化率和产物选择性。在这里，我们报告了一种通过调节界面水结构来调节 ECSH 活性和选择性的新策略。所获得的 PdCu 二十面体在 96.5% 的转化率下提供了显着提高的转化率和 98.5% 的烯烃选择性，并能维持约 100 小时的连续测试。证明源自二十面体孪晶结构的拉伸应变有助于形成界面水结构，特别是K +离子水合水（K·H 2 O）和2-配位氢键水（2-HB·H 2○）。我们还解读了界面水结构在 ECSH 性能中的神秘作用，其中 K·H 2 O 加速水分解产生 H广告，进而加速 ECSH 转化，而 2-HB·H 2 O 提高了烯烃的选择性。这些发现从晶格应变的角度为质子耦合氢化电催化剂设计中界面水结构的调整提供了见解。
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