Pd Supported on MIL-68(In)-Derived In2O3 Nanotubes as Superior Catalysts to Boost CO2 Hydrogenation to Methanol,ACS Catalysis

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Pd Supported on MIL-68(In)-Derived In2O3 Nanotubes as Superior Catalysts to Boost CO2 Hydrogenation to Methanol
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-11-02 , DOI: 10.1021/acscatal.0c03372
Zhongjie Cai ₁ , Jiajun Dai ₁ , Wen Li ₂ , Kok Bing Tan ₁ , Zhongliang Huang ₃ , Guowu Zhan ₃ , Jiale Huang ₁ , Qingbiao Li _{1,

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Affiliation

Utilization of CO₂ and its conversion to value-added chemicals are highly desirable to alleviate the environmental concerns caused by the massive anthropogenic CO₂ emission. Although In₂O₃/Pd have been employed as efficient catalysts for hydrogenation of CO₂ to methanol, the electronic effects by strong metal–support interaction (SMSI) between Pd and In₂O₃ are poorly understood, which is greatly affected by the morphology of In₂O₃. Herein, we use MIL-68(In) nanorod as a morphological template for the synthesis of hollow In₂O₃ nanotubes (h-In₂O₃) and the preparation of supported Pd catalysts for CO₂ hydrogenation to methanol. Interestingly, loading Pd on h-In₂O₃ showed a much higher performance than In₂O₃ with other morphologies, which exhibited almost unchanged CO₂ conversion of 10.5%, methanol selectively of 72.4%, and methanol space-time yield of 0.53 g_MeOH h^–1 g_cat^–1 over 100 h on stream at 3 MPa and 295 °C. After in-depth characterizations, we found that the different electronic properties of Pd species on In₂O₃ can be finely tuned by diverse synthetic conditions, which were responsible for high activity and stability. The molar fraction of Pd²⁺ species in the h-In₂O₃/Pd catalyst reached 67.6%, 3.2 times that of the In₂O₃@Pd catalyst (21.3%), due to the different surface chemistry of In₂O₃. Density function theory results indicated that the Pd donated more electrons to the curved In₂O₃ (222) surface than the pristine surface, and Pd²⁺ was critical to facilitate H₂ adsorption and formation of the surface oxygen vacancy. This work demonstrates that controlling the morphology of In₂O₃ can modify both the Pd electronic property and SMSI between Pd and In₂O₃, which are the origins of the high catalytic performance.

中文翻译：

Pd支撑在MIL-68（In）衍生的₂ O ₃纳米管中，作为促进CO ₂加氢成甲醇的高级催化剂

利用CO ₂并将其转化为增值化学品是非常需要的，以减轻由大量人为排放的CO ₂引起的环境问题。尽管In ₂ O ₃ / Pd已被用作将CO ₂加氢成甲醇的有效催化剂，但人们对Pd和In ₂ O ₃之间的强金属-载体相互作用（SMSI）产生的电子效应知之甚少，这受到了很大的影响。 In ₂ O _3的形貌。在这里，我们使用MIL-68（In）纳米棒作为形态模板，用于合成中空的In ₂ O ₃纳米管（h-In ₂ O ₃）和用于CO ₂加氢为甲醇的负载型Pd催化剂的制备。有趣的是，在h -In ₂ O ₃上负载Pd表现出比其他形态的In ₂ O ₃高得多的性能，其他形态的CO ₂转化率几乎不变，为10.5％，甲醇选择性为72.4％，甲醇时空产率为0.53。 g _MeOH h ^–1 g _cat^–1在3 MPa和295°C的条件下运行100 h以上。经过深入的表征，我们发现Pd物种在In ₂ O上的不同电子性质₃可以通过多种合成条件进行微调，这些合成条件具有很高的活性和稳定性。钯的摩尔分数²⁺在物种H-在₂ ö ₃ /钯催化剂达到67.6％，即在3.2倍₂ ö ₃ @Pd催化剂（21.3％），由于在不同的表面化学₂ ö ₃。密度函数理论结果表明，Pd向弯曲的In ₂ O ₃（222）表面贡献的电子比原始表面多，Pd ²⁺对于促进H ₂至关重要吸附并形成表面氧空位。这项工作表明，控制In ₂ O ₃的形态可以同时改变Pd和In ₂ O ₃之间的Pd电子性能和SMSI ，这是高催化性能的起源。

更新日期：2020-11-21

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