利用流动池将 CO2 高效电催化还原为 HCOOH 并将其与 5-羟甲基糠醛氧化耦合

IF 3.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-08-09 DOI:10.1002/aic.18562
Jing Ren, Zixian Li, Chenjun Ning, Shaoquan Li, Luming Zhang, Hengshuo Huang, Lirong Zheng, Young Soo Kang, Mingchuan Luo, Yufei Zhao
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引用次数: 0

摘要

在电催化二氧化碳还原(CO2ER)的各种产物中,HCOOH 是利润很高的一种。然而,阳极氧进化反应的动力学速度较慢,降低了整体能效,而热力学势能较低且动力学速度较快的电氧化反应可以取代阳极氧进化反应。在此,我们报告了一种将 CO2ER 与 5-羟甲基糠醛氧化反应(HMFOR)耦合的电解系统。我们设计了一种 BiOCl-CuO 催化剂,可在部分电流密度为 500 mA/cm2 且 FEHCOOH 高于 90% 和 700 mA/cm2 且 FEHCOOH 高于 80% 的条件下维持 CO2ER 转化为 HCOOH。原位和非原位 X 射线吸收精细结构被用来捕捉 CO2ER 过程中 BiOCl-CuO 向金属 Bi 和 Cu 的结构转变,CuO 的存在将促进这种转变,这一点得到了 DFT 计算的支持。将 HMFOR 与 CO2ER 相结合,我们同时实现了 95% 以上的 FEHCOOH 和 FEFDCA,为利用配对体系电合成高附加值产品提供了新的前景。
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High-efficient electrocatalytic CO2 reduction to HCOOH coupling with 5-hydroxymethylfurfural oxidation using flow cell

Among various products from electrocatalytic CO2 reduction (CO2ER), HCOOH is highly profitable one. However, the slow kinetics of anodic oxygen evolution reaction lowers overall energy efficiency, which can be replaced by an electro-oxidation reaction with low thermodynamic potential and fast kinetics. Herein, we report an electrolysis system coupling CO2ER with 5-hydroxymethylfurfural oxidation reaction (HMFOR). A BiOCl–CuO catalyst was designed to sustain CO2ER to HCOOH at partial current density of 500 mA/cm2 with FEHCOOH above 90% and 700 mA/cm2 with FEHCOOH above 80%. In situ and ex situ x-ray absorption fine structure was used to capture the structure transform of BiOCl–CuO into metallic Bi and Cu during CO2ER process, and the presence of CuO will promote this transformation which are supported by DFT calculations. Coupling HMFOR with CO2ER, we realize both FEHCOOH and FEFDCA above 95% simultaneously, providing new prospects vista for the electrosynthesis of value-added products from paired system.

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来源期刊
AIChE Journal
AIChE Journal 工程技术-工程:化工
CiteScore
7.10
自引率
10.80%
发文量
411
审稿时长
3.6 months
期刊介绍: The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.
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