Chow Cheuk-Fai, Ho Pui-Yu, Wong Wing-Leung, Lu Yu-Jing, Tang Qian, Gong Cheng-Bin
Department of Science and Environmental Studies , The Education University of Hong Kong , 10 Lo Ping Road, Tai Po , Hong Kong SAR , China . Email:
College of Chemistry and Chemical Engineering , Southwest University , Chong Qing , China.
Chem Sci. 2017 May 1;8(5):3812-3820. doi: 10.1039/c6sc05584b. Epub 2017 Mar 2.
Latent catalysts can be tuned to function smartly by assigning a sensing threshold using the displacement approach for targeted analytes. Three cyano-bridged bimetallic complexes were synthesized as "smart" latent catalysts through the supramolecular assembly of different metallic donors [Fe(CN)], [Fe(Bubpy)(CN)], and Fe(Bubpy)(CN) with a metallic acceptor [Cu(dien)]. The investigation of both their thermodynamic and kinetic properties on binding with toxic pollutants provided insight into their smart off-on catalytic capabilities, enabling us to establish a threshold-controlled catalytic system for the degradation of pollutants such as cyanide and oxalate. With these smart latent catalysts, a new catalyst displacement assay (CDA) was demonstrated and applied in a real wastewater treatment process to degrade cyanide pollutants in both domestic (level I, untreated) and industrial wastewater samples collected in Hong Kong, China. The smart system was adjusted to be able to initiate the catalytic oxidation of cyanide at a threshold concentration of 20 μM (the World Health Organization's suggested maximum allowable level for cyanide in wastewater) to the less harmful cyanate under ambient conditions.
通过使用针对目标分析物的置换方法设定传感阈值,可以调整潜在催化剂以实现智能功能。通过不同金属供体[Fe(CN)]、[Fe(Bubpy)(CN)]和Fe(Bubpy)(CN)与金属受体[Cu(dien)]的超分子组装,合成了三种氰基桥联双金属配合物作为“智能”潜在催化剂。对它们与有毒污染物结合的热力学和动力学性质的研究,深入了解了它们智能的开启-关闭催化能力,使我们能够建立一个用于降解氰化物和草酸盐等污染物的阈值控制催化系统。利用这些智能潜在催化剂,展示了一种新的催化剂置换分析方法(CDA),并将其应用于实际废水处理过程,以降解在中国香港收集的生活污水(一级,未处理)和工业废水样本中的氰化物污染物。该智能系统被调整为能够在20 μM的阈值浓度(世界卫生组织建议的废水中氰化物的最大允许水平)下引发氰化物在环境条件下催化氧化为危害较小的氰酸盐。