Reconstruction of the surface Bi3+ oxide layer on Bi2O2CO3: Facilitating electron transfer for enhanced photocatalytic degradation performance of antibiotics in water

IF 5.1 2区材料科学 Q1 MATERIALS SCIENCE, CERAMICS

Ceramics International Pub Date : 2024-12-15 DOI:10.1016/j.ceramint.2024.10.132

Yu Fang, Liu Hong, Yang Dai, Qing Xiang, NianBing Zhang, Jiaojiao Li

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Abstract

The advancement and meticulous design of functional photocatalysts exhibiting exceptional photocatalytic redox activity represent a pivotal approach to mitigating the dual challenges of environmental pollution and energy scarcity. In this study, we elucidate the construction of a Bi₂O₂CO₃ catalytic system capable of inhibiting oxidative electron transfer through the attenuation of homogeneous Bi⁰ particle formation, achieved through the judicious modulation of solvent ratios. This innovative architecture possesses a distinctive active site and enhances interfacial Bi-O electron transfer pathways via exposure to oxidized Bi³⁺. Upon photoexcitation, the Bi₂O₂CO₃ catalytic system undergoes structural distortions in its excited state that facilitate forbidden radiative relaxation, thereby fostering long-lived charge separation states. Remarkable catalytic activity was demonstrated in the remediation of pollutants, encompassing auto-oxidation and the catalytic degradation of superoxide radicals (•O₂⁻) and holes (h⁺). Notably, the effective degradation of tetracycline hydrochloride (TCH) in aqueous media reached an impressive 86 % under simulated visible light irradiation, accompanied by a reaction rate constant 3.08 times superior to that of the 5-Bi/Bi₂O₂CO₃ counterpart. Theoretical analyses revealed that the oxidized state of Bi₂O₂CO₃ exhibits a crystal structure with significant electron trapping capability, undergoing pronounced apparent relaxation phenomena on its surface while demonstrating an enhanced adsorption affinity for H₂O and O₂. The potential degradation mechanisms were rigorously investigated through High-performance liquid chromatography (HPLC-MS), elucidating the photodegradation pathways and intermediates of TC. This work may serve as a distinct paradigm for the rational design of novel photocatalysts aimed at fostering sustainable environmental remediation and advancing energy innovation.

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重构 Bi2O2CO3 表面的 Bi3+ 氧化层：促进电子转移以提高水中抗生素的光催化降解性能

开发和精心设计具有卓越光催化氧化还原活性的功能性光催化剂，是缓解环境污染和能源短缺双重挑战的关键方法。在本研究中，我们阐明了如何构建一种 Bi2O2CO3 催化体系，该体系能够通过明智地调节溶剂比例来减少均质 Bi0 粒子的形成，从而抑制氧化电子转移。这种创新结构具有独特的活性位点，通过接触氧化 Bi3+，增强了界面 Bi-O 电子转移途径。光激发时，Bi2O2CO3 催化系统的激发态会发生结构畸变，从而促进禁止辐射弛豫，进而形成长寿命的电荷分离态。该催化系统在污染物修复方面具有显著的催化活性，包括自动氧化以及催化降解超氧自由基（-O2-）和空穴（h+）。值得注意的是，在模拟可见光照射下，水介质中盐酸四环素（TCH）的有效降解率达到了惊人的 86%，反应速率常数是 5-Bi/Bi2O2CO3 对应物的 3.08 倍。理论分析表明，Bi2O2CO3 的氧化态晶体结构具有显著的电子捕获能力，其表面出现明显的表观弛豫现象，同时对 H2O 和 O2 的吸附亲和力增强。通过高效液相色谱法（HPLC-MS）对潜在的降解机制进行了严格研究，阐明了 TC 的光降解途径和中间产物。这项工作可作为合理设计新型光催化剂的独特范例，旨在促进可持续的环境修复和推动能源创新。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Ceramics International 工程技术-材料科学：硅酸盐

CiteScore

9.40

自引率

15.40%

发文量

4558

审稿时长

25 days

期刊介绍： Ceramics International covers the science of advanced ceramic materials. The journal encourages contributions that demonstrate how an understanding of the basic chemical and physical phenomena may direct materials design and stimulate ideas for new or improved processing techniques, in order to obtain materials with desired structural features and properties. Ceramics International covers oxide and non-oxide ceramics, functional glasses, glass ceramics, amorphous inorganic non-metallic materials (and their combinations with metal and organic materials), in the form of particulates, dense or porous bodies, thin/thick films and laminated, graded and composite structures. Process related topics such as ceramic-ceramic joints or joining ceramics with dissimilar materials, as well as surface finishing and conditioning are also covered. Besides traditional processing techniques, manufacturing routes of interest include innovative procedures benefiting from externally applied stresses, electromagnetic fields and energetic beams, as well as top-down and self-assembly nanotechnology approaches. In addition, the journal welcomes submissions on bio-inspired and bio-enabled materials designs, experimentally validated multi scale modelling and simulation for materials design, and the use of the most advanced chemical and physical characterization techniques of structure, properties and behaviour. Technologically relevant low-dimensional systems are a particular focus of Ceramics International. These include 0, 1 and 2-D nanomaterials (also covering CNTs, graphene and related materials, and diamond-like carbons), their nanocomposites, as well as nano-hybrids and hierarchical multifunctional nanostructures that might integrate molecular, biological and electronic components.