Multistep catalytic abiotic CO2 conversion to sugars through C1 intermediates

• 成果类型: Article
• 署名作者: Solanda, Nathan; Luoa, Jie; Maulanab, Arifin Luthfi; Feijooa, Julian; Joc, Hye-Jin; Oddoa, Alexander M.; Shanb, Yu; Wanga, Tianle; Leea, Geonhui; Choib, Jihoon; Huynha, Wei-Shan; Guzmana, Maria Fonseca; Jayasinghea, Lihini; Zhub, Cheng; Yanga, Yao; Yanga, Peidong
• 署名单位: University of California System; University of California Berkeley; University of California System; University of California Berkeley; University of California System; University of California Berkeley; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; Zhejiang University; Seoul National University (SNU); Northwestern University; Cornell University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-10078
• DOI: 10.1073/pnas.2514826122
• 发表日期: 2025-08-26
• 关键词: formaldehyde; chemistry; carbenes; hydrogen

摘要

Carbon dioxide (CO2) to multicarbon (Cn) upgrading for commodity chemicals, fuel production, or artificial food synthesis using renewable energy input is a golden target for researchers in sustainable carbon emission reduction. Here, we explore and analyze a flexible modular roadmap for the task, utilizing sequential electro-, photo-, and organocatalysis to develop a strategy for CO2 conversion using the key and elusive formaldehyde precursor of interest for sugar generation. We study the electrochemical carbon dioxide reduction reaction to methanol in a flow cell and its discontinuous photooxidation to formaldehyde (PMOR) with excellent selectivity. Utilizing a highly active N-heterocyclic carbene catalyst enables tunable generation of C4-C6 aldoses without undesirable byproducts, with carbon conversion yield reaching 60 to 80% for desired pentose, tetrose, and triose product mixtures and over 20% for hexose. This approach presents a roadmap for CO2 valorization, aiming to bridge carbon waste streams with sustainable sugar synthesis and opening broad avenues for green chemical production.