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用于同时平衡去除六价铬和四环素的碳化钛(TiC)基纤维状二氧化硅催化剂的工程电子能带结构

Engineered electronic band structure of titanium carbide (TiC)-based fibrous silica catalyst for balanced simultaneous removal of hexavalent chromium and tetracycline.

作者信息

Hassan N S, Jalil A A, Sawal M H, Sofi M H M, Salwa V A, Rajendran Saravanan

机构信息

Centre of Hydrogen Energy, Institute of Future Energy, UTM Johor Bahru, Johor, 81310, Malaysia.

Centre of Hydrogen Energy, Institute of Future Energy, UTM Johor Bahru, Johor, 81310, Malaysia; Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia, UTM Johor Bahru, 81310, Johor, Malaysia; Chemical Engineering Department, Institut Teknologi Sepuluh Nopember, Kampus ITS Sukolilo, Surabaya, 60111, Indonesia.

出版信息

J Environ Manage. 2025 Aug;389:126082. doi: 10.1016/j.jenvman.2025.126082. Epub 2025 Jun 3.

DOI:10.1016/j.jenvman.2025.126082
PMID:40466307
Abstract

Simultaneous removal of tetracycline (TC) and hexavalent chromium (Cr(VI)) from wastewater is limited by low photocatalytic efficiency and complex catalyst recovery. This study investigates titanium carbide (TiC)-based fibrous silica KAUST Catalysis Centre (KCC-1) composites for the visible-light-driven removal of TC and Cr(VI), focusing on the effects of calcination, TiC loading (1-5 wt%), and synthesis method. Uncalcined TiC/KCC-1 outperformed the calcined catalyst due to its higher surface area, anatase content, and stronger TiC-support interaction. Among loadings, 3TiC/KCC-1 achieved the highest removal (68 % Cr(VI), 66 % TC), while one-pot synthesized TiC/KCC-1 (1P) showed superior performance (73 % Cr(VI), 72 % TC), lower energy demand (731 kWh/m), and cost (USD 36.7) compared to the impregnated catalyst (TiC/KCC-1 (IM)). Enhanced activity is attributed to its narrow band gap (1.7 eV), efficient charge separation, and favorable band positions. Electrochemical studies revealed TiC/KCC-1 (1P) improved charge transfer and reduced resistance. Mechanistically, TiC/KCC-1 (1P) directs photogenerated electrons toward Cr(VI) reduction via its +0.70 eV conduction band, while its +2.4 eV valence band supports TC oxidation through hydroxyl radical formation. In contrast, TiC/KCC-1 (IM) suffers from electron competition and insufficient oxidative potential due to its less favorable band positions. These findings underscore TiC/KCC-1 (1P) as a promising, green, energy-efficient photocatalyst for multi-contaminant wastewater treatment.

摘要

从废水中同时去除四环素(TC)和六价铬(Cr(VI))受到光催化效率低和催化剂回收复杂的限制。本研究考察了基于碳化钛(TiC)的纤维状二氧化硅沙特阿卜杜拉国王科技大学催化中心(KCC-1)复合材料用于可见光驱动去除TC和Cr(VI)的性能,重点研究了煅烧、TiC负载量(1-5 wt%)和合成方法的影响。未煅烧的TiC/KCC-1由于其较高的比表面积、锐钛矿含量和更强的TiC-载体相互作用,性能优于煅烧后的催化剂。在不同负载量中,3TiC/KCC-1实现了最高的去除率(68%的Cr(VI),66%的TC),而一锅法合成的TiC/KCC-1(1P)表现出更优的性能(73%的Cr(VI),72%的TC),与浸渍法制备的催化剂(TiC/KCC-1(IM))相比,其能量需求更低(731 kWh/m),成本也更低(36.7美元)。活性增强归因于其窄带隙(1.7 eV)、有效的电荷分离和有利的能带位置。电化学研究表明,TiC/KCC-1(1P)改善了电荷转移并降低了电阻。从机理上讲,TiC/KCC-1(1P)通过其+0.70 eV的导带将光生电子导向Cr(VI)的还原,而其+2.4 eV的价带通过形成羟基自由基来支持TC的氧化。相比之下,TiC/KCC-1(IM)由于其不太有利的能带位置而存在电子竞争和氧化电位不足的问题。这些发现突出了TiC/KCC-1(1P)作为一种用于多污染物废水处理的有前景的、绿色的、节能的光催化剂。

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