原位开发 3D Cu-CeO2 催化剂选择性用于生物质呋喃化合物电催化加氢,ACS Catalysis

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原位开发 3D Cu-CeO2 催化剂选择性用于生物质呋喃化合物电催化加氢
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-09-15 , DOI: 10.1021/acscatal.3c03363
Giancosimo Sanghez de Luna ₁ , Patrick Zeller _{2,

3} , Eylül Öztuna _{2,

3} , Francesco Maluta _{1,

4} , Andrea Canciani _{1,

4} , Francesca Ospitali ₁ , Phuoc H. Ho ₁ , Alessandro Paglianti ₁ , Axel Knop-Gericke _{2,

5} , Giuseppe Fornasari _{1,

4} , Juan J. Velasco-Vélez _{2,

5,

6} , Patricia Benito _{1,

4}

Affiliation

可再生电力驱动的电催化氢化生物质衍生的呋喃化合物在温和的反应条件下产生生物聚合物（聚氨酯）前体。由于电二聚作用的影响，广泛使用的银和铜电催化剂未能在浓电解质中将醛选择性转化为醇。在此，我们提出了基于3D CeO ₂的催化剂，用于将5-羟甲基糠醛（HMF）电解质（0.02、0.05和0.10 M）电催化氢化为2,5-双羟甲基呋喃（BHMF）。采用电沉积方法在Cu开孔泡沫上涂覆CeO _{2 。}电催化剂的异位表征表明它们是由 CeO _2制成的层含有Cu物质。铜从泡沫到涂层的迁移是在电沉积过程中开始的，而电还原条件则引发了铜颗粒的形成。X射线吸收光谱的原位表征证明Ce ⁴⁺到Ce ³⁺的还原发生在施加阴极电位之后。此外，在实验过程中铜物质被还原为Cu ^{0 。}_{部分还原的CeO 2}和Cu颗粒的组合不仅提供了选择性反应位点，而且增加了电极的电导率。因此，原位生长的 Cu-CeO ₂电催化剂促进了浓度更高的 0.10 M HMF 电解质的选择性电催化氢化，在 -0.51 V vs RHE 下的性能优于之前报道的 AgCu 材料。

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In Situ Development of a 3D Cu-CeO2 Catalyst Selective in the Electrocatalytic Hydrogenation of Biomass Furanic Compounds

The renewable electricity-driven electrocatalytic hydrogenation of biomass-derived furanic compounds produces biopolymer (polyurethane) precursors under mild reaction conditions. The widely used Ag and Cu electrocatalysts failed in the selective conversion of the aldehyde into the alcohol in concentrated electrolytes due to the contribution of the electrodimerization. Herein, we proposed 3D CeO₂-based catalysts for the electrocatalytic hydrogenation of 5-hydroxymethylfurfural (HMF) electrolytes (0.02, 0.05, and 0.10 M) to 2,5-bishydroxymethylfuran (BHMF). An electrodeposition approach was adopted to coat CeO₂ on Cu open-cell foams. The ex-situ characterization of electrocatalysts revealed that they were made of a CeO₂ layer containing Cu species. The migration of Cu from the foam to the coating started during the electrodeposition, while the electroreduction conditions provoked the formation of Cu particles. The in situ characterization by X-ray absorption spectroscopy evidenced that the Ce⁴⁺ to Ce³⁺ reduction occurred just after the application of the cathodic potential; moreover, copper species were reduced to Cu⁰ during the experiments. The combination of partially reduced CeO₂ and Cu particles not only provided selective reaction sites but also increased the electrical conductivity of the electrode. Consequently, the in situ-developed Cu-CeO₂ electrocatalysts promoted the selective electrocatalytic hydrogenation of the more concentrated 0.10 M HMF electrolytes, overperforming previously reported AgCu materials at −0.51 V vs RHE.

更新日期：2023-09-15

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