Simultaneous Glycolate and Hydrogen Generation Enabled by Unassisted Photocathode-Anode Cells

IF 26 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Dongfeng Du, Yumeng Han, Peixuan Liu, Linxiao Wu, Bin Shao, Jingshan Luo
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Abstract

Photoelectrochemical (PEC) water splitting has emerged as a highly promising solar-driven technology for sustainable chemical synthesis. However, this photosynthesis-inspired approach is limited by slow oxygen evolution kinetics. Herein, a bias-free, energy-saving PEC system for simultaneous glycolate and hydrogen production is reported. A highly efficient PdAu catalyst on Ni foam is developed for the upgrading of ethylene glycol (EG) derived from polyethylene terephthalate (PET) plastics, which shows a high performance for electrochemical glycolate production with a low onset potential of 0.25 V vs the reversible hydrogen electrode (RHE) and a high Faradaic efficiency (FE) of 95.6% at 100 mA cm−2. When coupled with a cuprous oxide (Cu2O) photocathode, the constructed solar-driven PEC-HER//EGOR device achieves a photocurrent density of up to 5.6 mA cm−2 at zero applied bias, owing to the lower potential requirement of EG oxidation than oxygen evolution reaction. Moreover, it has nearly unity hydrogen FE and 94.8% glycolate FE at 1 h of unbiased operation, showing great potential in continuous and simultaneous hydrogen production and PET-derived EG valorization without any additional bias or expensive chemicals. This work demonstrates a straightforward, energy-efficient, and environmentally benign solar-to-chemical conversion approach for integrating environmental remediation and PEC synthesis.

Abstract Image

无辅助光电阴极-阳极电池同时生成乙醇酸和氢
光电化学(PEC)水分解是一种非常有前途的太阳能驱动的可持续化学合成技术。然而,这种受光合作用启发的方法受到缓慢的析氧动力学的限制。本文报道了一种无偏置、节能的同时生产乙醇酸和氢气的PEC系统。开发了一种高效的PdAu催化剂,用于镍泡沫塑料中聚对苯二甲酸乙二醇酯(PET)的升级,该催化剂在可逆氢电极(RHE)下的起始电位低至0.25 V,在100 mA cm−2下的法拉第效率(FE)高达95.6%,具有良好的电化学乙醇酸盐生产性能。当与氧化亚铜(Cu2O)光电阴极耦合时,由于EG氧化比析氧反应需要更低的电位,构建的太阳能驱动PEC-HER//EGOR装置在零施加偏置下实现了高达5.6 mA cm - 2的光电流密度。此外,在无偏置操作1小时时,它具有几乎统一的氢FE和94.8%的乙醇酸FE,在连续和同时制氢和pet衍生的EG增值方面显示出巨大的潜力,而无需任何额外的偏置或昂贵的化学品。这项工作展示了一种简单、节能、环保的太阳能-化学转化方法,用于整合环境修复和PEC合成。
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来源期刊
Advanced Energy Materials
Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
41.90
自引率
4.00%
发文量
889
审稿时长
1.4 months
期刊介绍: Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.
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