Rich electron delocalization structure in carbon nitride inducing radical transfer for high-performance photocatalytic uranyl reduction

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Energy Pub Date : 2024-08-23 DOI:10.1002/cey2.636
Zhangmeng Liu, Yayao Li, Shuaiqi Yao, Runchao Zhou, Guiting Lin, Yunzhi Fu, Qixin Zhou, Wei Wang, Weijie Chi
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Abstract

Investigating the activation of the persulfate process through heterogeneous carbonaceous catalysts to expedite the reduction of uranyl ions (U(VI)) is imperative. The primary hurdle involves understanding the transfer and distribution of photogenerated carriers during the reduction process in this intricate system and deciphering the role of activated groups in promoting reduction efficiency. In this study, we strategically regulate the structure of polymeric carbon nitride to promote the N-doped state, thereby facilitating delocalization electron enrichment. The resulting active sites effectively activate peroxyl disulfate (PDS), generating radicals that expedite the selective reduction of U(VI). This strategic approach mitigates the inherent disadvantage of the short half-life of free radicals in persulfate-based advanced oxidation processes. As a consequence of our endeavors and with the simultaneous presence of PDS and hydrogen peroxide, we achieve an exceptional photoreduction efficiency of 100% within a remarkably short period of 20 min. This breakthrough presents a high-efficiency application with significant potential for addressing the pollution associated with uranyl-containing wastewater. Our findings not only contribute to the fundamental understanding of AOPs but also offer a practical solution with implications for environmental remediation.

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氮化碳中诱导自由基转移的丰富电子致焦结构可实现高性能光催化铀酰还原
研究通过异质碳质催化剂激活过硫酸盐过程以加快铀酰离子(U(VI))的还原过程势在必行。首要的障碍是了解光生载流子在这一错综复杂的系统中还原过程中的转移和分布,并破译活化基团在促进还原效率方面的作用。在这项研究中,我们对聚合氮化碳的结构进行了策略性调节,以促进 N 掺杂状态,从而促进电子富集。由此产生的活性位点可有效激活过氧二硫酸盐(PDS),产生自由基,从而加速 U(VI)的选择性还原。这种策略性方法缓解了基于过硫酸盐的高级氧化过程中自由基半衰期短的固有缺点。经过努力,在 PDS 和过氧化氢同时存在的情况下,我们在极短的 20 分钟内实现了 100% 的卓越光还原效率。这一突破为解决含铀废水污染问题提供了一种具有巨大潜力的高效应用。我们的研究成果不仅有助于从根本上理解 AOPs,还为环境修复提供了实用的解决方案。
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来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
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Issue Information Cover Image, Volume 6, Number 10, October 2024 Back Cover Image, Volume 6, Number 10, October 2024 Interface and doping engineering of V2C-MXene-based electrocatalysts for enhanced electrocatalysis of overall water splitting Issue Information
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