Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-08-12 , DOI: 10.1016/j.cej.2020.126613 Kai Zhang , Ziwen Chang , Xubiao Luo , Lixia Yang , Junjun Pei , Shenglian Luo
Selective extraction of target metal ions from contaminated water is always the concern in the absorbent application. Herein, a palladium ion-imprinted polymer (Pd-IIP-AHTB) absorbent was designed and fabricated through radical-induced polymerization of Schiff based functional monomer (3-Allyl-2-hydroxybenzaldehyde thiosemicarbazone, AHTB) to selectively recover Pd2+ from water. Pd-IIP-AHTB shows a high distribution coefficient Kd (850.46 mL g−1) which is up to 110 times higher than that of interference metal ion like Zn(II). pH 3.0 was chosen as an optimum pH in the adsorption operation. The maximum adsorption capacity on Pd-IIP-AHTB is 60 mg/g, which is 2 times that of the non-imprinted polymer (NIP) (30.33 mg/g) at 25 °C. Dubinin-Ashtakhov (DA) based site energy distribution model (F(E*)) confirms that more accessible sites are binding with Pd2+ on Pd-IIP-AHTB than NIP (Q0(F(E*)Pd-IIP-AHTB > Q0(F(E*)NIP, and E0*Pd-IIP-AHTB > E0*NIP). We elucidated a new Pd2+ adsorption mechanism that involves a strong coordination interaction between Pd2+ and binding site (X->CN and Y->CS) in a 3-D Pd-IIP-AHTB with memory effect cavity. Notably, the strong coordination enables the specific spatial transfer PdCl42− to [X-Pd-Y] in aqueous solution by fixed bed adsorption experiments verification, and no Cl− ions are retained on the absorbent. This finding provides new insight into the recovery of highly purified Pd on fixed bed packed Pd-IIP-AHTB absorbents and renewal hydrochloric acid solution in practical application.
中文翻译:
在具有足迹腔的3D钯离子印迹聚合物中,通过强配位相互作用,空间空间转移PdCl 4 2-到[X-Pd-Y]
从吸收水中选择性地提取目标金属离子一直是吸收剂应用中关注的问题。本文中,通过自由基诱导的席夫基功能单体(3-烯丙基-2-羟基苯甲醛硫代半脲,AHTB)自由基聚合,设计并制造了钯离子印迹聚合物(Pd-IIP-AHTB)吸收剂,以选择性地从水中回收Pd 2+。 。Pd-IIP-AHTB显示出较高的分配系数K d(850.46 mL g -1),它比Zn(II)等干扰金属离子的110倍高。选择pH 3.0作为吸附操作中的最佳pH。在25°C下,Pd-IIP-AHTB的最大吸附容量为60 mg / g,是非印迹聚合物(NIP)(30.33 mg / g)的2倍。基于Dubinin-Ashtakhov(DA)的站点能量分布模型(F(E *))证实,与NIP相比,更多可访问的站点与Pd-IIP-AHTB上的Pd 2+结合的是N Q(Q 0(F(E *)Pd-IIP- AHTB > Q 0(F(E *)NIP和E 0 * Pd-IIP-AHTB > E 0 *NIP)。我们阐明了一种新的Pd 2+吸附机制,该机制涉及具有记忆效应腔的3-D Pd-IIP-AHTB中Pd 2+与结合位点(X->CN和Y->CS)之间的强配位相互作用。值得注意的是,强的协调使特定空间传递的PdCl 4 2-对[X PD-Y]在通过固定床吸附实验验证水溶液,和无氯-离子保留在吸收剂上。这一发现为在固定床装填的Pd-IIP-AHTB吸收剂中回收高纯Pd以及在实际应用中更新盐酸溶液提供了新的见解。