湖南大学王双印团队报道了电催化促进甲醇热催化脱氢生产高纯H₂和CO。相关研究成果于2024年4月1日发表在《美国化学会杂志》。

甲醇制氢是一种能源可持续的乙醇生产方式，但通常会导致大量二氧化碳排放。将甲醇选择性转化为H₂和有价值的化学原料提供了一种有前景的策略。然而，它受到苛刻的操作条件和低转换效率的限制。

该文中，研究人员通过在双功能Ru/C催化剂上耦合热催化甲醇脱氢和电催化氢氧化，实现了从甲醇高效生产高纯度H₂和CO。电催化能够加速C–H的裂解，并降低阳极处的氢气分压，从而推动化学平衡，显著增强甲醇脱氢。此外，设计了双层Ru/C+Pd/C电极以减轻CO中毒并促进氢氧化。因此，通过在200°C下整合0.4 V的外加电池电压，获得了高纯度（99.9%）的高产率H₂（558.54 mmol h^–1 g^–1），优于传统的热催化和电催化过程，并且CO是阳极的主要产物。

该项工作为高效生产H₂以及从甲醇进行有价值的化学合成，提供了一条新途径。

附：英文原文

Title: Electrocatalysis Boosts the Methanol Thermocatalytic Dehydrogenation for High-Purity H2 and CO Production

Author: Yujie Wu, Gen Huang, Shiqian Du, Miaoyu Li, Qie Liu, Yangyang Zhou, Zuyao Jiang, Xiaorong Zhu, Yuqing Wang, Tehua Wang, Li Tao, Shuangyin Wang

Issue&Volume: April 1, 2024

Abstract: Hydrogen production from methanol represents an energy-sustainable way to produce ethanol, but it normally results in heavy CO2 emissions. The selective conversion of methanol into H2 and valuable chemical feedstocks offers a promising strategy; however, it is limited by the harsh operating conditions and low conversion efficiency. Herein, we realize  efficient high-purity H2 and CO production from methanol by coupling the thermocatalytic methanol dehydrogenation with electrocatalytic hydrogen oxidation on a bifunctional Ru/C catalyst. Electrocatalysis enables the acceleration of C–H cleavage and reduces the partial pressure of hydrogen at the anode, which drives the chemical equilibrium and significantly enhances methanol dehydrogenation. Furthermore, a bilayer Ru/C + Pd/C electrode is designed to mitigate CO poisoning and facilitate hydrogen oxidation. As a result, a high yield of H2 (558.54 mmol h–1 g–1) with high purity (99.9%) was achieved by integrating an applied cell voltage of 0.4 V at 200 °C, superior to the conventional thermal and electrocatalytic processes, and CO is the main product at the anode. This work presents a new avenue for efficient H2 production together with valuable chemical synthesis from methanol.

DOI: 10.1021/jacs.3c13240

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.3c13240