Coproduction of Glyceric Acid and Glycolic Acid from Biomass-Based Sugars over a Ru/Co3O4 Catalyst,ACS Catalysis

当前位置： X-MOL 学术 › ACS Catal. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Coproduction of Glyceric Acid and Glycolic Acid from Biomass-Based Sugars over a Ru/Co3O4 Catalyst
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-05-01 , DOI: 10.1021/acscatal.4c00782
Yancheng Liu ₁ , Shiwei Zhou ₁ , Xiaoyan Wang ₂ , Jingying Qin ₁ , Changwei Hu ₁ , Jianmei Li ₁

Affiliation

α-Hydroxyl acid production from biomass has emerged as a promising approach for biomass valorization but remains a long-standing challenge due to limited productivity. Herein, we established an innovative strategy for the coproduction of glyceric and glycolic acids from pentose feedstocks. Ru/Co₃O₄ catalyst, possessing tunable Ruⁿ⁺/Ru⁰ ratio and abundant oxygen vacancy, was found to promote the total yield of glyceric acid and glycolic acid (up to 65.9 C-mol % with a ∼1:1 molar ratio based on the initial carbon in the feedstock, the highest value among the state-of-the-art advances) at a mild temperature (70 °C). The results of the isotopic tracing experiments confirmed that xylose underwent C2–C3 cleavage, yielding glyceraldehyde and glycolaldehyde intermediates, which could be oxidized to produce glyceric acid and glycolic acid, respectively. In combination with density functional theory (DFT) calculations, it was revealed that Ruⁿ⁺ and Ru⁰ with an appropriate Ruⁿ⁺/Ru⁰ ratio, in addition to oxygen vacancies, made a pronounced cooperative contribution to achieve complicated cascade reactions. Ruⁿ⁺ was proven to be more favorable for xylose adsorption via the interaction with the −C═O, thereby accelerating the ring-opening reaction and C2–C3 cleavage, while Ru⁰, together with oxygen vacancies, mainly contributed to the activation of O₂ to produce active oxygen species that facilitated the immediate oxidation of intermediates. The results of this work may provide useful insights into catalyst design and potential directions to maximize carbon utilization in biomass valorization.

中文翻译：

Ru/Co3O4 催化剂上生物质糖联产甘油酸和乙醇酸

利用生物质生产α-羟基酸已成为生物质增值的一种有前景的方法，但由于生产力有限，仍然是一个长期存在的挑战。在此，我们制定了利用戊糖原料联产甘油和乙醇酸的创新策略。 Ru/Co ₃ O ₄催化剂具有可调的Ru ^{n +} /Ru ⁰比和丰富的氧空位，被发现可以提高甘油酸和乙醇酸的总产率（高达65.9 C-mol %，摩尔比为~1:1）在温和的温度（70°C）下，基于原料中的初始碳的比例（最先进的技术中的最高值）。同位素示踪实验的结果证实，木糖发生C2-C3裂解，产生甘油醛和乙醇醛中间体，它们可以分别被氧化产生甘油酸和乙醇酸。结合密度泛函理论（DFT）计算，发现Ru ^{n +}和Ru ⁰具有适当的Ru ^{n +} /Ru ⁰比例，除了氧空位之外，还对实现复杂的级联反应做出了显着的协同贡献。 Ru ^{n +}被证明通过与-C=O的相互作用更有利于木糖的吸附，从而加速开环反应和C2-C3裂解，而Ru ⁰与氧空位一起主要有助于木糖的活化。 O ₂产生活性氧，促进中间体的立即氧化。这项工作的结果可能为催化剂设计和最大化生物质增值中碳利用率的潜在方向提供有用的见解。

更新日期：2024-05-01

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南