Total hydrogenation of bio-derived furans over supported Ru subnanoclusters prepared via amino acid-assisted deposition,Green Chemistry

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Total hydrogenation of bio-derived furans over supported Ru subnanoclusters prepared via amino acid-assisted deposition
Green Chemistry ( IF 9.3 ) Pub Date : 2020/01/02 , DOI: 10.1039/c9gc02943e
Yang Qian _{1,

2,

3,

4,

5} , Ze-Jun Li _{1,

2,

3,

4,

5} , Xian-Long Du _{5,

6,

7,

8} , Qi Zhang _{1,

2,

3,

4,

5} , Yi Zhao _{1,

2,

3,

4,

5} , Yong-Mei Liu _{1,

2,

3,

4,

5} , Yong Cao _{1,

2,

3,

4,

5}

Affiliation

Development of a highly efficient and robust catalyst with reduced usage of noble metals is extremely desirable for selective hydrogenations of furan-containing bio-based feedstocks, which represents an attractive and sustainable alternative to petrochemical resources. Herein, we describe a new type of well-dispersed Ru subnanoclusters (ca. 0.50 wt%) supported on commercial P25 TiO₂ material obtained from a facile and effective amino acid-assisted deposition–precipitation strategy. The as-synthesized catalyst exhibits superior catalytic activity and selectivity for direct hydrogenation of industrially important furfural as well as a range of structurally diverse bio-based furanic compounds to their corresponding fully hydrogenated derivatives. An average turnover frequency (ATOF) value as high as 367 h⁻¹ at 80 °C and 4 MPa H₂ is obtained, which is the highest reported value. This catalyst also shows stable furfural total hydrogenation in 5 reaction cycles conducted at 80 °C (52 mmol-scale, turnover number up to 12 500). In terms of the kinetic and structural characterizations, the key performances of the ultrasmall Ru clusters are proposed to mainly originate from an enhanced number of unsaturated surface Ru atoms and change in local coordination environment. Our work highlights the importance of the subnanometric size of Ru clusters in the advancement of efficient and affordable approaches towards bio-based chemical production.

中文翻译：

通过氨基酸辅助沉积制备的负载型Ru亚簇上生物衍生呋喃的总氢化

对于含呋喃的生物基原料的选择性加氢，开发一种减少贵金属使用量的高效，坚固的催化剂是非常需要的，这代表了石化资源的一种有吸引力且可持续的替代方法。在这里，我们描述了一种新型的分散在商业P25 TiO ₂上的Ru分散的亚纳米簇（约0.50 wt％）通过简便有效的氨基酸辅助沉积沉淀策略获得的材料。合成后的催化剂对工业上重要的糠醛以及一系列结构多样的生物基呋喃化合物直接加氢成其相应的完全氢化的衍生物具有优异的催化活性和选择性。在80°C和4 MPa H _2下，平均周转频率（ATOF）值高达367 h ^-1是获得的，这是最高的报告值。该催化剂还显示出在80°C（52 mmol规模，周转数高达12 500）下进行的5个反应循环中稳定的糠醛总氢化。在动力学和结构表征方面，超小Ru团簇的关键性能主要来自不饱和表面Ru原子数量的增加和局部配位环境的变化。我们的工作强调了Ru团簇的亚纳米尺寸在推动高效且负担得起的生物基化学生产方法方面的重要性。

更新日期：2020-02-13

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