Insight into the Effect of Dual Active Cu0/Cu+ Sites in a Cu/ZnO-Al2O3 Catalyst on 5-Hydroxylmethylfurfural Hydrodeoxygenation,ACS Sustainable Chemistry & Engineering

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Insight into the Effect of Dual Active Cu0/Cu+ Sites in a Cu/ZnO-Al2O3 Catalyst on 5-Hydroxylmethylfurfural Hydrodeoxygenation
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-09-16 , DOI: 10.1021/acssuschemeng.0c05235
Qian Wang _{1,

2,

3} , Zhi Yu _{1,

2} , Junting Feng _{1,

2} , Paolo Fornasiero ₃ , Yufei He _{1,

2} , Dianqing Li _{1,

2}

Affiliation

The production of biofuel 2,5-dimethylfuran (DMF) from an important biomass platform of 5-hydroxymethyl furfural (HMF) involves a complicated reaction pathway due to the competition of C═O hydrogenation and C–O hydrogenolysis; however, the dependence of formed intermediates and catalytic sites needs to be further identified. Herein, we constructed a highly efficient and selective Cu/ZnO-Al₂O₃ catalyst via reduction of a CuZnAl-layer double hydroxide (LDH) precursor, aimed for studying the effect of Cu⁰/Cu⁺ species on forming different intermediates and their synergetic promotional effect on HMF hydrodeoxygenation. As expected, the dependence of formation of different intermediates on the Cu⁺/Cu⁰ ratio was observed; notably, Cu/ZnO-Al₂O₃ with higher Cu⁺/Cu⁰ ratio finally gave 90.1% DMF selectivity at 100% HMF conversion, more selective than CuNi/Al₂O₃ (59.6%) and Cu/MgO-Al₂O₃ (75.8%) references. By a combined study of in situ IR experiments, the observed correlation between the reaction intermediates and the Cu⁰/Cu⁺ site suggests that Cu⁰ tends to adsorb the C═O bond as well as hydrogen molecule, while the Cu⁺ site is preferable to adsorb and activate the C–O bond. With the synergy of dual active sites, the Cu/ZnO-Al₂O₃ catalyst showed both high activity and selectivity to DMF. This work provides deep insight into the nature of active Cu species in multiple functional group biomass platform transformation.

中文翻译：

了解Cu / ZnO-Al ₂ O ₃催化剂中双重活性Cu ⁰ / Cu ^+位点对5-羟甲基糠醛加氢脱氧的影响

由5-羟甲基糠醛（HMF）的重要生物量平台生产生物燃料2,5-二甲基呋喃（DMF）涉及复杂的反应途径，这是由于C═O加氢和CO氢解的竞争所致。然而，需要进一步确定所形成的中间体和催化位点的依赖性。本文中，我们通过还原CuZnAl层双氢氧化物（LDH）前驱体构建了一种高效且选择性的Cu / ZnO-Al ₂ O ₃催化剂，旨在研究Cu ⁰ / Cu ⁺物种对形成不同中间体及其混合物的影响。对HMF加氢脱氧的协同促进作用。如预期的那样，不同中间体的形成对Cu ⁺ / Cu ⁰的依赖性观察比例；值得注意的是，具有更高Cu ⁺ / Cu ⁰比的Cu / ZnO-Al ₂ O ₃最终在100％HMF转化率下具有90.1％DMF选择性，比CuNi / Al ₂ O ₃（59.6％）和Cu / MgO-Al ₂更具选择性O ₃（75.8％）参考。通过原位红外实验的组合研究，观察到的反应中间体与Cu ⁰ / Cu ⁺位点之间的相关性表明，Cu ⁰倾向于吸附C═O键以及氢分子，而Cu ⁺位点则更可取吸附并激活C–O键。借助双重活性位点的协同作用，Cu / ZnO-Al₂ O ₃催化剂显示出高活性和对DMF的选择性。这项工作提供了深入的洞察活性铜物种在多官能团生物量平台转化中的性质。

更新日期：2020-10-12

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