Novel Insights into the Configurations of Lead(II)-Benzohydroxamic Acid Coordination Compounds in Aqueous Solution: A Combined Experimental and Computational Study
Novel Insights into the Configurations of Lead(II)-Benzohydroxamic Acid Coordination Compounds in Aqueous Solution: A Combined Experimental and Computational Study
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DOI：
10.20944/preprints201806.0110.v2
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发表时间：
2018-07
影响因子：
2.8
通讯作者：
Jianyong He;Hai-sheng Han;Chenyang Zhang;Yue-hua Hu;Dandan Yuan;Mengjie Tian;Daixiong Chen;Wei Sun
中科院分区：
文献类型：
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作者：
Jianyong He;Hai-sheng Han;Chenyang Zhang;Yue-hua Hu;Dandan Yuan;Mengjie Tian;Daixiong Chen;Wei Sun
采用紫外-可见（UV-Vis）光谱、电喷雾电离-质谱（ESI-MS）以及考虑溶剂化效应的第一性原理密度泛函理论（DFT）等实验方法，对新型铅（II）-苯并异羟肟酸（Pb（II）-BHA）水溶液捕收剂配合物进行了表征. Job图表明，Pb（BHA）+首先形成单配位，随后形成更高配位数的配合物。此外，Pb（II）-BHA物种可以彼此聚集以形成复杂的结构，例如Pb（BHA）2或高度复杂的络合物。ESI-MS结果验证了Pb-（BHA）n= 1，2在不同pH值下的存在。此外，第一性原理计算表明Pb（BHA）+是最稳定的结构，Pb（BHA）+中的Pb原子将作为攻击亲核试剂的活性位.这些结果对进一步阐明Pb（II）-BHA络合物在选矿过程中的吸附机理具有重要意义。
Novel collector lead(II)-benzohydroxamic acid (Pb(II)-BHA) complexes in aqueous solution were characterized by using experimental approaches, including Ultraviolet-visible (UV-Vis) spectroscopy and electrospray ionization–mass spectrometry (ESI-MS), as well as first-principle density functional theory (DFT) calculations with consideration for solvation effects. The Job plot delineated that a single coordinated Pb(BHA)+ should be formed first, and the higher coordination number complexes can be formed subsequently. Moreover, the Pb(II)-BHA species can aggregate with each other to form complicated structures, such as Pb(BHA)2 or highly complicated complexes. ESI-MS results validated the existence of Pb-(BHA)n=1,2 under different solution pH values. Further, the first-principles calculations suggested that Pb(BHA)+ should be the most stable structure, and the Pb atom in Pb(BHA)+ will act as an active site to attack nucleophiles. These findings are meaningful to further illustrate the adsorption mechanism of Pb(II)-BHA complexes in mineral processing.