首页|桥联配体对钛凝胶吸附砷锑性能的影响及机制

桥联配体对钛凝胶吸附砷锑性能的影响及机制

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针对钛凝胶吸附剂中桥联配体与吸附性能之间的关系不明问题,本文对比考察了由11种配体(有机羧酸类、醇胺类以及双酮类)合成的钛凝胶材料吸附砷(As)、锑(Sb)的性能。乙酰丙酮(AcAc)作为桥联配体合成的钛凝胶材料表现出优异的As、Sb去除能力,其对As(Ⅲ)、As(Ⅴ)、Sb(Ⅲ)和Sb(Ⅴ)的吸附容量分别达到了 329、461、584、805 mg·g-1(以钛计),吸附速率分别比无配体组提高了 10。1、8。1、11。5、1。9倍。各类配体对钛凝胶吸附容量的提升效果相当,但对吸附速率提升效果差异明显。有机羧酸类配体调控后对As、Sb吸附速率仅为AcAc的30%—60%,而丁二酮等弱配体调控后几乎没有提升吸附速率。与其他配体相比,AcAc的配位能力介于丁二酮和酒石酸、三乙醇胺等强配体之间,其适中的配位能力兼顾了制备过程中抑制钛快速水解和吸附过程中新活性位点的快速释放特性。当AcAc中心碳或端基碳被甲基取代后,烯醇式AcAc的含量以及配位能力降低,进而减弱材料的砷锑吸附性能。
Effects and mechanism of bridging ligands on the adsorption performance for arsenic and antimony removal by titanium xerogel
To clarity the relationship between the structure of bridging ligands and the adsorption performance,a series of titanium xerogels were synthesized with 11 ligands(organic carboxylic acids,alcohol-amines,and diketones)and their performance for arsenic and antimony removal was investigated.The titanium xerogel synthesized with acetylacetone(AcAc)as a bridging ligand showed an excellent adsorption performance:the adsorption capacities to As(Ⅲ),As(Ⅴ),Sb(Ⅲ),and Sb(Ⅴ)were 329,461,584 and 805 mg·g-1(in titanium),respectively,and the adsorption rates were 10.1,8.1,11.5 and 1.9 times higher than that of the xerogel without organic ligand.All the tested ligands had comparable effects on the adsorption capacity,but led to significant differences in the adsorption rate.The xerogels with organic carboxylic acid ligands adsorbed As and Sb at rates of only 30%—60%of that with AcAc,while weak ligand,such as butanedione,had negligible effect on the adsorption rate.Compared with other ligands,AcAc had a moderate coordination capacity between butanedione and strong ligands(e.g.,tartaric acid and triethanolamine),which balanced the inhibition of rapid hydrolysis of titanium during synthesis and the quick release of new active sites during adsorption.When the hydrogen at the central or terminal carbon of AcAc was substituted by methyl groups,the content of the enolic form and consequently the coordination ability were reduced,which in turn weakened the adsorption performance.

heavy metal pollutiontitanium xerogel adsorbentacetylacetoneligandssol-gel

张皓铭、周畅、张国洋、张淑娟

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南京大学环境学院污染控制与资源化研究国家重点实验室,南京,210023

重金属污染 钛凝胶吸附剂 乙酰丙酮 配体 溶胶凝胶法

科技部重点研发计划国家自然科学基金

2019YFC040830222106068

2024

环境化学
中国科学院生态环境研究中心

环境化学

CSTPCD北大核心
影响因子:1.049
ISSN:0254-6108
年,卷(期):2024.43(4)
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