​中科大Nat. Commun.: 低配位Cu增强Cu/Cu2O整流界面效应，实现CO2-多碳醇转化

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电化学CO2还原(CER)生产增值化学品和燃料是应对日益严重的能源和环境危机的有效策略。由于C2+醇具有广阔的市场潜力和高能量密度，因此成为CER的热门产品。双相Cu/Cu2O催化剂由于对*CO有较高的吸附倾向性，而且C-C或C2-C偶联的能类较低，在合成C2+醇方面具有良好的性能。然而，由于碳氢化合物中间体的不稳定性和Cu氧化状态变化，Cu/Cu2O催化剂在抑制C2H3O*的解吸和提高醇的产量方面面临重大障碍。因此，需要制定可行的策略来修饰改性Cu/Cu2O以保持Cu基催化剂氧化状态和提高CO2性能。


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近日，中国科学技术大学章根强课题组以Cl掺杂的氧化亚铜(Cl-Cu2O)和纯Cu2O为前驱体，通过原位电化学重构策略调制了Cu中心配位环境，在Cu/Cu2O界面上构建低配位Cu中心并诱导非对称电子扰动和更快的电子交换，从而促进C-C偶联和*CO-COH与C2H2O*中间体加氢生成C2+醇。
理论计算和实验结果表明，低配位CuL/Cu2O催化剂提高CER性能的几个要素为：首先，CuL/Cu2O催化剂内部的低配位和不对称电子聚集是其界面区快速电子交换和增强中间体吸附的主要原因；此外，Cu+/Cu0的优良电导率和电荷差促进了C-C或C-C2偶联的亲核或亲电加成反应过程。
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最重要的是，在增强的界面上，Cu+离子与Cu之间的快速电子转移会引起晶格收缩，从而抑制了负责稳定Cu+离子化学价的剩余氧原子的损失；而Cu/Cu2O区域保证了氧烃中间体的顺利吸附和解吸，以及偶联行为。还有就是，电化学重构Cl-Cu2O产生了大量的氧空位和残余Cl缺陷，为吸附的中间体提供了丰富的自由电子和锚定点。
这些结果共同作用于低配位CuL/Cu2O Mott-Schottky催化剂，显著提高C2+醇的选择性。具体而言，C2+醇的法拉第效率和能量效率分别达到64.15%和39.32%，并表现出50 h以上的稳定性(J= 200 mA cm-2，FE>50%)。
Low-coordinated copper facilitates the *CH2CO affinity at enhanced rectifying interface of Cu/Cu2O for efficient CO2-to-multicarbon alcohols conversion. Nature Communications, 2024. DOI: 10.1038/s41467-024-49247-4




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