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壳聚糖水凝胶锚定酞菁负载金属纳米粒子:用于污染物还原和制氢的双功能催化剂。

Chitosan hydrogel anchored phthalocyanine supported metal nanoparticles: Bifunctional catalysts for pollutants reduction and hydrogen production.

机构信息

Chemistry Department, Faculty of Science, King Abdulaziz University, P.O. Box 80203, Jeddah, 21589, Saudi Arabia.

Chemistry Department, Faculty of Science, King Abdulaziz University, P.O. Box 80203, Jeddah, 21589, Saudi Arabia; Department of Chemistry, Bacha Khan University, Charsadda, P.O. Box 24420, KP, Pakistan.

出版信息

Environ Pollut. 2023 Jun 15;327:121524. doi: 10.1016/j.envpol.2023.121524. Epub 2023 Mar 30.

Abstract

Metal nanoparticles possess high catalytic activity in various organic transformation reactions. A catalyst must be recovered and re-used effectively and economically to lower the overall reaction cost. The recovery of a catalyst remains a challenge due to their extreme small size. In this research work, catalytic metal nanoparticles were synthesized on Zn-phthalocyanine (ZnPc) and chitosan hydrogel (CH) composite which acts as catalyst support. The ZnPc-CH support facilitate the easy recovery of the loaded metal nanoparticles. Metal nanoparticles (M) based on Cu, Ag, Ni, Co and Fe were decorated inside and on ZnPc-CH hydrogel surface. The developed M@ZnPc-CH were utilized for the enhanced selective reduction of toxins and hydrogen production by methanolysis and hydrolysis of NaBH. Effective catalytic reduction and hydrogen generation was successfully achieved with Co@ZnPc-CH and ZnPc-CH. Under optimized conditions, Co@ZnPc-CH showed complete reduction of 4-nitrophenol (4-NP) in 8.0 min with the fast 4-NP reduction kinetics (K = 0.611 min). Among the developed catalysts, ZnPc-CH showed fast H generation with high H generation rate (HGR = 4100 mLgmin) under optimized conditions. Metal leaching from Co@ZnPc-CH was negligible during recycling of the catalyst, suggesting that it could be implemented to 4-NP treatment from real water samples. Similarly, ZnPc-CH could produce same quantity of H throughout 4 continuous cycles of durability testing without any deactivation and leaching and ZnPc-CH showed high stability, indicating the effectiveness of the catalyst to be applied for H production on large scale.

摘要

金属纳米粒子在各种有机转化反应中具有高催化活性。为了降低整体反应成本,必须有效地和经济地回收和再利用催化剂。由于其极小的尺寸,催化剂的回收仍然是一个挑战。在这项研究工作中,催化金属纳米粒子被合成在 Zn-酞菁(ZnPc)和壳聚糖水凝胶(CH)复合材料上,该复合材料作为催化剂载体。ZnPc-CH 载体有利于负载金属纳米粒子的容易回收。基于 Cu、Ag、Ni、Co 和 Fe 的金属纳米粒子(M)被修饰在 ZnPc-CH 水凝胶内部和表面上。开发的 M@ZnPc-CH 被用于增强通过甲醇解和 NaBH 水解对毒素的选择性还原和氢气生成。Co@ZnPc-CH 和 ZnPc-CH 成功地实现了有效的催化还原和氢气生成。在优化条件下,Co@ZnPc-CH 显示出在 8.0 分钟内完全还原 4-硝基苯酚(4-NP),具有快速的 4-NP 还原动力学(K=0.611 min)。在所开发的催化剂中,ZnPc-CH 在优化条件下显示出快速的 H 生成和高的 H 生成速率(HGR=4100 mLgmin)。在催化剂的循环回收过程中,Co@ZnPc-CH 中的金属浸出可以忽略不计,这表明它可以用于从实际水样中处理 4-NP。同样,ZnPc-CH 可以在 4 个连续的耐久性测试循环中产生相同数量的 H,而没有任何失活和浸出,ZnPc-CH 表现出高稳定性,表明该催化剂在大规模生产 H 方面的有效性。

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