Ru(0) 催化生物质中 C-O 和 C-C 键完全裂解生成天然气,ACS Catalysis

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Ru(0) 催化生物质中 C-O 和 C-C 键完全裂解生成天然气
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-04-25 , DOI: 10.1021/acscatal.2c00310
Zhiwen Ren _{1,

2} , Xiaoqin Si ₁ , Jiali Chen _{1,

3} , Xiaobing Li _{1,

2} , Fang Lu ₁

Affiliation

作为天然丰富的可再生资源，生物质能对能源格局产生重大影响。将可再生生物质转化为天然气特别令人着迷，但由于结构复杂，仍然具有挑战性。在这里，我们开发了一种催化策略，通过在 Ru(0) 上完全裂解 C-O 和 C-C 键，将木质纤维素生物质高效转化为天然气。X射线光电子能谱表明Ru原子被还原为金属态。此外，Ru(0) 促进了生物质中 C-O 和 C-C 键的催化裂解。对于具有各种C-O和C-C键的异山梨醇，气体碳收率高达93.5%，CH _{4为85.4 mol%}和 7.1 mol% 的 C2-C4 烃在气碳产物分布中，周转频率高达 206.8 h ^-1。研究了原料生物质的进一步转化以获得气体产品中 90.0 mol% 的 CH ₄。对反应途径的研究表明，连位羟基是催化裂解C-C键的基本前提。此外，与仲羟基相邻的 C-C 键的断裂比伯羟基的断裂要困难得多，这表明 C-O 和 C-C 键的催化断裂的能垒较低。因此，与伯羟基相邻的 C-C 键的逐步断裂可能是生物质催化转化为天然气的主要贡献。

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Catalytic Complete Cleavage of C–O and C–C Bonds in Biomass to Natural Gas over Ru(0)

Being the naturally abundant renewable resource, biomass plays a significant influence on the energy landscape. The transformation of renewable biomass into natural gas is particularly fascinating but remains challenging due to the structural complexity. Here, we developed a catalytic strategy for the high-efficiency transformation of lignocellulosic biomass into natural gas through the complete cleavage of C–O and C–C bonds over Ru(0). X-ray photoelectron spectra showed that Ru atoms were reduced to the metallic state. Moreover, Ru(0) facilitated the catalytic cleavage of C–O and C–C bonds in the biomass. For isosorbide with various C–O and C–C bonds, the gas carbon yield reached up to 93.5% with 85.4 mol % of CH₄ and 7.1 mol % of C2–C4 hydrocarbons in gas carbon product distribution, and the turnover frequencies were up to 206.8 h^–1. The further conversion of raw biomass was investigated to obtain 90.0 mol % of CH₄ in gas products. Investigation on the reaction pathway revealed that the vicinal hydroxyl group was the fundamental prerequisite for the catalytic cleavage of the C–C bond. Moreover, the cleavage of the C–C bond adjacent to the secondary hydroxyl group was much more difficult than that of the primary hydroxyl group which revealed the low energy barrier for the catalytic cleavage of C–O and C–C bonds. Thus, the stepwise cleavage of the C–C bond adjacent to the primary hydroxyl group might be the main contribution to the catalytic transformation of the biomass into natural gas.

更新日期：2022-04-25

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