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基于木质素的非均相光催化剂直接从海水中生成 HO。

Lignin-Supported Heterogeneous Photocatalyst for the Direct Generation of HO from Seawater.

机构信息

Department of Chemistry, Universiteit Antwerpen, Antwerp 2020, Belgium.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 10691, Sweden.

出版信息

J Am Chem Soc. 2022 Feb 16;144(6):2603-2613. doi: 10.1021/jacs.1c10786. Epub 2022 Feb 7.

Abstract

The development of smart and sustainable photocatalysts is in high priority for the synthesis of HO because the global demand for HO is sharply rising. Currently, the global market share for HO is around 4 billion US$ and is expected to grow by about 5.2 billion US$ by 2026. Traditional synthesis of HO via the anthraquinone method is associated with the generation of substantial chemical waste as well as the requirement of a high energy input. In this respect, the oxidative transformation of pure water is a sustainable solution to meet the global demand. In fact, several photocatalysts have been developed to achieve this chemistry. However, 97% of the water on our planet is seawater, and it contains 3.0-5.0% of salts. The presence of salts in water deactivates the existing photocatalysts, and therefore, the existing photocatalysts have rarely shown reactivity toward seawater. Considering this, a sustainable heterogeneous photocatalyst, derived from hydrolysis lignin, has been developed, showing an excellent reactivity toward generating HO directly from seawater under air. In fact, in the presence of this catalyst, we have been able to achieve 4085 μM of HO. Expediently, the catalyst has shown longer durability and can be recycled more than five times to generate HO from seawater. Finally, full characterizations of this smart photocatalyst and a detailed mechanism have been proposed on the basis of the experimental evidence and multiscale/level calculations.

摘要

开发智能和可持续的光催化剂对于 HO 的合成至关重要,因为全球对 HO 的需求正在急剧上升。目前,HO 的全球市场份额约为 40 亿美元,预计到 2026 年将增长约 52 亿美元。传统的蒽醌法合成 HO 会产生大量的化学废物,并且需要高能量输入。在这方面,通过氧化转化纯水是满足全球需求的可持续解决方案。事实上,已经开发了几种光催化剂来实现这一化学转化。然而,地球上 97%的水是海水,其中含有 3.0-5.0%的盐分。盐在水中的存在会使现有的光催化剂失活,因此,现有的光催化剂很少显示出对海水的反应活性。考虑到这一点,已经开发了一种可持续的异质光催化剂,由水解木质素衍生而来,在空气中直接从海水中生成 HO 具有优异的反应活性。事实上,在这种催化剂的存在下,我们已经能够实现 4085 μM 的 HO。便利地,该催化剂表现出更长的耐久性,并且可以在海水中重复使用五次以上来生成 HO。最后,根据实验证据和多尺度/水平计算提出了这种智能光催化剂的全面特性和详细的机制。

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