One-Pot Synthesis of Tensile-Strained PdRuCu Icosahedra toward Electrochemical Hydrogenation of Alkene,ChemElectroChem

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One-Pot Synthesis of Tensile-Strained PdRuCu Icosahedra toward Electrochemical Hydrogenation of Alkene
ChemElectroChem ( IF 3.5 ) Pub Date : 2021-08-12 , DOI: 10.1002/celc.202100827
Kaili Zhu ₁ , Xudong Xu ₁ , Mengqiu Xu ₂ , Ping Deng ₂ , Wenbo Wu ₂ , Wei Ye ₃ , Zihui Weng ₂ , Yue Su ₂ , Huijie Wang ₂ , Fei Xiao ₂ , Zeping Fang ₂ , Peng Gao ₄

Affiliation

Electrochemical hydrogenation (ECH) uses electricity to drive proton (H⁺) reduction for hydrogenation, which can greatly reduce energy supply and environmental pollution, representing an ideal alternative to traditional thermal hydrogenation. In this work, we put forward tensile-strained PdRuCu alloy to promote ECH. Tensile strain promotes the adsorption of C=C by changing the d-band center. Meanwhile, alloying Ru and Cu into Pd lattice facilitates hydrogenation by weakening Pd−H bonding. Therefore, PdRuCu icosahedra display excellent ECH performance of 2-methyl-3-buten-2-ol (MBE) with specific activity of 227.4 μmol_MBE nm⁻² min⁻¹ at −0.3 V versus reversible hydrogen electrode (RHE), about 16.1 and 10.5 times higher than that of commercial Pd/C and Ru/C, respectively. In addition, PdRuCu icosahedra was excellent in the scaling up of substrate concentration combined with anisyl alcohol oxidation to produce high-value added anisaldehyde at anode. This work provides a guideline for the rational design of highly active and durable metallic catalyst in ECH.

中文翻译：

拉应变PdRuCu二十面体的一锅法合成烯烃电化学加氢

电化学加氢（ECH）利用电力驱动质子（H ⁺）还原进行加氢，可大大减少能源供应和环境污染，是传统热加氢的理想替代方案。在这项工作中，我们提出了拉伸应变 PdRuCu 合金来促进 ECH。拉伸应变通过改变d 带中心促进 C=C 的吸附。同时，将 Ru 和 Cu 合金化到 Pd 晶格中通过削弱 Pd-H 键来促进氢化。因此，PdRuCu 二十面体显示出 2-methyl-3-buten-2-ol (MBE) 的优异 ECH 性能，比活性为 227.4 μmol _MBE nm ^-2 min ^-1在 -0.3 V与可逆氢电极（RHE），分别比商用 Pd/C 和 Ru/C 高约 16.1 和 10.5 倍。此外，PdRuCu 二十面体在扩大底物浓度与茴香醇氧化相结合以在阳极产生高附加值的茴香醛方面表现出色。这项工作为 ECH 中高活性和耐用金属催化剂的合理设计提供了指导。

更新日期：2021-10-13

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