介孔酸性 SiO2–Al2O3 载体促进镍加氢催化芳族 LOHC 化合物中的氢储存,ACS Sustainable Chemistry & Engineering

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介孔酸性 SiO2–Al2O3 载体促进镍加氢催化芳族 LOHC 化合物中的氢储存
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-11-11 , DOI: 10.1021/acssuschemeng.2c04978
Hwiram Jeong ₁ , Tae Wan Kim ₁ , Minseok Kim ₁ , Gi Bo Han ₂ , Byunghun Jeong ₃ , Young-Woong Suh _{1,

4}

Affiliation

过渡金属催化剂对于实现基于可逆加氢和脱氢的液态有机氢载体（LOHC）系统至关重要。为了获得与迄今为止主要使用的贵金属催化剂相当的加氢活性，需要将催化剂成分混合在一起以改善吸附和动力学。对于芳族 LOHC（单苄基甲苯）氢化中的镍催化，_本文_使用异丙醇_铝和烷基三乙氧基硅烷（C n _TES，其中n = 3、8 , 和 18). 尽管所有制备的催化剂中的 Ni 粒径相似，但 Ni/MSA_C 的加氢活性_{n TES 与 C}_n TES的烷基取代基长度呈火山型关系，其中 Ni/MSA_C₈ TES 显示出比负载在介孔氧化铝上的 Ni 催化剂高 2 倍的活性。观察到的火山趋势归因于受路易斯酸度影响的芳香底物的吸附，更重要的是，氢吸附在位于混合 SiO₂ –Al₂ O₃区域附近的 Ni 物种上，该区域具有 Brønsted 酸质子以促进H₂溢出。此外，MSA_C_n的介孔TES 有助于反应物和产物的轻松传输。因此，这些催化剂特性将在单个 Ni 催化剂体中得到很好的平衡，以提高 LOHC 加氢性能。

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Mesoporous Acidic SiO2–Al2O3 Support Boosts Nickel Hydrogenation Catalysis for H2 Storage in Aromatic LOHC Compounds

Transition-metal catalysts are essential to realize a liquid organic hydrogen carrier (LOHC) system based on reversible hydrogenation and dehydrogenation. To attain comparable hydrogenation activity to noble metal catalysts mainly used so far, catalyst constituents need to be blended together toward improved adsorption and kinetics. For nickel catalysis in the hydrogenation of aromatic LOHC (monobenzyltoluene), mesoporous SiO₂–Al₂O₃ (MSA) supports are herein prepared by solvent-deficient precipitation using aluminum isopropoxide and alkyltriethoxysilane (C_nTES, in which n = 3, 8, and 18). Although Ni particle sizes are similar in all of the prepared catalysts, the hydrogenation activity of Ni/MSA_C_nTES is in a volcano-shaped relationship with the length of the alkyl substituent of C_nTES, where Ni/MSA_C₈TES shows 2-fold superior activity to the Ni catalyst supported on mesoporous alumina. The observed volcano trend is attributed to the adsorption of aromatic substrates affected by Lewis acidity and, more significantly, the adsorption of hydrogen on the Ni species located in the vicinity of the mixed SiO₂–Al₂O₃ domains having Brønsted acidic protons for promoted H₂ spillover. Moreover, the mesopores of MSA_C_nTES contribute to the facile transport of the reactant and the product. Therefore, these catalyst characteristics would be well balanced in single Ni catalyst bodies for boosted LOHC hydrogenation performance.

更新日期：2022-11-11

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