Controlled Synthesis of Water–Soluble Pt Nanoclusters and Their Co–Catalysis with RuO2–IrO2 for Electrochemical Degradation of Tetracycline

Controlled Synthesis of Water–Soluble Pt Nanoclusters and Their Co–Catalysis with RuO2–IrO2 for Electrochemical Degradation of Tetracycline
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水溶性Pt纳米团簇的可控合成及其与RuO2-IrO2的协同催化电化学降解四环素

DOI:
10.1016/j.seppur.2022.121323
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发表时间:
2022-05
影响因子:
8.6
通讯作者:
Junfeng Niu
Junfeng Niu
中科院分区:
工程技术1区
文献类型:
--
作者:
Jianjun Zhou;Fan Pan;Tian Wang;Yujie Zhang;Qiaofeng Yao;Chao Zhu;Yunqing Zhu;Hongrui Ma;Junfeng Niu

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·采用一步法制备了超小、原子级精确的Pt 8纳米团簇。·硫醇保护的Pt 8纳米团簇由于热稳定的Pt-S键合而表现出优异的抗烧结性能。· Pt 8纳米团簇与RuO 2 -IrO 2共催化体系对四环素的电催化降解具有较高的活性和稳定性。提出了四环素的电催化降解机理。铂原子级工程实现最小的铂剂量和最大的电催化性能是一种有效的电催化剂设计策略。本文采用一步法合成了L-半胱氨酸保护的超小Pt 8纳米团簇,并与RuO 2 -IrO 2共催化,电催化降解四环素.得益于巯基配体的保护和原子级的精细结构,该纳米簇电催化剂不仅具有优异的抗烧结性能,而且对四环素的降解表现出优异的电催化活性(降解率为100%,矿化率为73.8%)和高稳定性,显示了Pt NCs催化剂在实际工艺条件下工业电化学氧化的应用潜力。此外,通过液相色谱-质谱联用技术对四环素电催化降解过程中的中间产物进行分析,提出了四环素电催化降解的机理。该工作为提高Pt基电催化剂的电催化性能提供了一种有效的原子级工程策略,这对抗生素污染废水的环境修复具有重要意义。
• A ultrasmall and atomically precise Pt 8 nanoclusters was prepared by a one–step route. • Thiol–protected Pt 8 nanoclusters exhibited outstanding anti–sintering property due to the thermally stable Pt–S bonding. • Pt 8 nanoclusters co-catalyzed with RuO 2 –IrO 2 showed high electrocatalytic activity and stability for tetracycline degradation. • The electrocatalytic degradation mechanism of tetracycline was proposed. Pt atomic–level engineering to achieve minimal Pt dosage and maximum electrocatalytic performance is an effective electrocatalyst design strategy. Here a one–step route to synthesize ultrasmall L–Cysteine–protected Pt 8 nanoclusters (NCs) and co–catalysis with RuO 2 –IrO 2 for electrocatalytic degradation of tetracycline is shown. Benefiting from sulfhydryl ligand protection and atomic–precision structure, the nanocluster electrocatalyst not only showed outstanding anti–sintering properties but also exhibited excellent electrocatalytic activity (degradation efficiency of 100% and mineralization rate of 73.8%) and high stability for tetracycline degradation, demonstrating the application potentials of Pt NCs catalyst for industrially electrochemical oxidation under practical technical conditions. Moreover, the electrocatalytic degradation mechanism of tetracycline was proposed by determining intermediates using liquid chromatography–mass spectrometry. This work provides an efficient atomic–level engineering strategy to enhance the electrocatalytic performance of Pt–based electrocatalysts, which has important implications for environmental remediation of antibiotic contaminated wastewater.
原位热辅助负载单分散 Pt 纳米团簇到 CdS 纳米花上,实现高效光催化析氢
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