On-Demand Catalytic Platform for Glycerol Upgrade and Utilization

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2025-02-04 DOI:10.1021/jacs.4c13603
Jianguo Zhao, Shuai Hao, Panpan Zhao, Jiao Ding, Rui Li, He Zhang, Shaojun Dong
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Abstract

Surplus byproducts generated during biomass exploitation, such as glycerol from biodiesel manufacturing, seriously undermine the credibility of renewable energy policies. Here, we establish an on-demand catalytic platform for the upgrade and utilization of glycerol via photoelectro-bioelectro-heterogeneous coupling catalysis. Combining theoretical descriptors, specifically the highest occupied molecular orbital energy levels and dual local softness values, along with systematic experimental validation, we demonstrated the reaction activity of glycerol and its upgraded products on BiVO4 photoelectrodes. Glyceric acid was identified as the optimal biofuel candidate through monohydroxyl oxidation of glycerol. Coupling the preferential upgrading of glycerol to glyceric acid by night and its reuse as biofuel by day, a hybrid biophotoelectrochemical system delivered an open-circuit voltage of 0.89 ± 0.02 V and a maximum power density of 0.41 ± 0.03 mW cm–2 with stable diurnal operation for over 10 days. This successful model construction provides valuable insights into the strategic integration of multiple energy sources and the exploration of coupling-catalytic platforms, charting new territory for the next-generation sustainable energy systems.

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甘油升级与利用按需催化平台
生物质开发过程中产生的剩余副产品,如生物柴油制造过程中产生的甘油,严重破坏了可再生能源政策的可信度。在此,我们建立了一个按需催化平台,通过光电-生物电非均相耦合催化对甘油进行升级和利用。结合理论描述符,特别是最高已占据分子轨道能级和双局部柔软度值,以及系统的实验验证,我们证明了甘油及其升级产物在BiVO4光电极上的反应活性。通过甘油的单羟基氧化,确定了甘油酸是最佳的生物燃料候选物。结合夜间将甘油优先升级为甘油酸和白天将其用作生物燃料的特性,该混合生物光电电化学系统可提供0.89±0.02 V的开路电压和0.41±0.03 mW cm-2的最大功率密度,并可稳定运行超过10天。这一成功的模型构建为多种能源的战略整合和耦合催化平台的探索提供了有价值的见解,为下一代可持续能源系统开辟了新的领域。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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