High-throughput discovery of organic working solutions enabling radical photochemistry for scalable H2O2 production

IF 37.1 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Joule Pub Date : 2026-08-05 DOI:10.1016/j.joule.2026.102603

Hyekyung Cho,Zahid Ullah,Sunil Kumar,Solhee Kim,Bolormaa Bayarkhuu,Xin Zhou,Yungui Li,Seunghyeon Kim,Moon Son,Jaeshik Chung,Jeehye Byun

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Abstract

Photocatalytic hydrogen peroxide (H2O2) production offers a sustainable and decentralized route for on-site chemical supply. However, conventional heterogeneous photocatalysis is constrained by single-photon events and surface charge recombination. Here, we report a photosensitizer-driven radical pathway in optimized organic working solutions (OWSs), enabling photochemical H2O2 generation beyond the single-photon limit. Using a data-driven framework integrating high-throughput screening and machine learning, 184 OWS combinations (5,888 experiments) were evaluated to uncover structure-performance relationships and identify an optimal formulation. The optimized OWS achieved an apparent quantum yield of 219.1%, consistent with a light-driven radical chain mechanism. A 1 L photoreactor produced 291 mM H2O2 with >99.9% purity and stable operation for 30 h. Donor regeneration and life-cycle analysis further support environmental and economic advantages over the anthraquinone process. This work establishes a generalizable platform for advancing solar-to-chemical production.

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高通量有机工作解决方案的发现，实现了可扩展H2O2生产的自由基光化学

光催化过氧化氢（H2O2）生产为现场化学品供应提供了可持续和分散的途径。然而，传统的非均相光催化受到单光子事件和表面电荷复合的限制。在这里，我们报道了在优化的有机工作溶液（OWSs）中光敏剂驱动的自由基途径，使光化学H2O2产生超过单光子限制。使用集成高通量筛选和机器学习的数据驱动框架，评估了184个OWS组合（5,888个实验），以揭示结构-性能关系并确定最佳配方。优化后的OWS表观量子产率达到219.1%，符合光驱动自由基链机制。一个1 L的光反应器产生291 mM的H2O2，纯度为bb0 99.9%，稳定运行30小时。供体再生和生命周期分析进一步支持了比蒽醌工艺更环保和经济的优势。这项工作为推进太阳能化工生产建立了一个可推广的平台。

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来源期刊

Joule Energy-General Energy

CiteScore

53.10

自引率

2.00%

发文量

198

期刊介绍： Joule is a sister journal to Cell that focuses on research, analysis, and ideas related to sustainable energy. It aims to address the global challenge of the need for more sustainable energy solutions. Joule is a forward-looking journal that bridges disciplines and scales of energy research. It connects researchers and analysts working on scientific, technical, economic, policy, and social challenges related to sustainable energy. The journal covers a wide range of energy research, from fundamental laboratory studies on energy conversion and storage to global-level analysis. Joule aims to highlight and amplify the implications, challenges, and opportunities of novel energy research for different groups in the field.