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掺磷PdNi催化剂的合成及其电催化脱氯机理研究
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Study on Preparation and Electrocatalytic Dechlorination Mechanism of phosphorus-doped Pd/NiP Nanoparticles
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    采用一步法合成含磷掺杂的Pd/NiP三元合金材料,其透射电子显微镜图、场发射 扫描电子显微镜图以及X射线光电子能谱图等结果显示,合成的Pd/NiP材料为直径(4.4 ±1.0) nm的超细纳米颗粒. 循环伏安结果显示该材料具有优异的电化学性能,Pd/NiP纳米颗粒中Pd 的电化学活性比表面积(ECSA)为42.11 m2 /g,是商业Pd/C纳米颗粒的1.5倍;Pd/NiP材料对4- 氯苯酚(4-CP)显示出优异的电催化脱氯活性,直接电化学还原脱氯和间接电催化脱氯加氢两 种途径均参与到 4-CP的电催化脱氯过程中 . 同时,伏安特性分析显示,直接电化学还原脱氯 过程中的电子转移系数(k)远小于 0.5,表明 C-Cl键的裂解遵循同步离解电子转移机理 . 研究 表明,掺杂Ni和P原子引起的协同效应和压缩应变显著增强了Pd生成与储存氢原子的能力, 同时有效抑制了氢气析出反应(HER),进而提升了电催化还原脱氯效率. 电解实验结果显示, 1.02 mg 该材料对 2 mmol/L 4-CP 的脱氯效率在 360 min 内可达到 87.5%,表观速率常数为 0.005 7 min-1,展现了极强的催化脱氯活性 . 三次循环实验结果显示,其脱氯效率仍达到 70% 以上,表明该材料具有较好稳定性 . 本工作为掺磷双金属纳米颗粒的合成提供了一种简便策 略,同时为电催化脱氯过程提供了一种良好的催化材料,为脱氯机理研究提供了重要参考.

    Abstract:

    Phosphorus doped PdNi nanoparticles were prepared by one-pot synthesis method,which was care? fully characterized by transmission electron microscope,scanning electron microscopy and X-ray photoelectron spectroscopy methods,showing an ultrafine particle size with a diameter of(4.4 ±1.0)nm. A cyclic voltammetry study demonstrated this material exhibited an excellent electrochemical property with an electrochemically active sur? face area(ECSA)of Pd at 42.11 m2 /g,which was 1.5 times higher than its commercial Pd/C counterparts. Pd/NiP nanoparticles showed a remarkable electrocatalytic dechlorination activity,in which direct electron transfer and indi? rect atomic hydrogen mediated electron transfer two pathways simultaneously occurred during the dehalogenation pro? cess. Meanwhile,voltammetric analyses showed that the electron transfer coefficient(k)was much smaller than 0.5, suggesting the dissociative electron transfer(DET)to the C-Cl bond of 4-CP following the concerted DET mecha? nism. Results indicated that the synergistic effect of trimetallic alloy and the compressive strain caused by the doping of Ni and P atoms markedly promoted the generation and retainment capacities of the adsorbed atomic hydrogen (H*ads)and the absorbed atomic hydrogen(H*abs),and effectively inhibited the hydrogen evolution reaction, thereby enhancing the electrocatalytic dechlorination efficiency. That was advantageous to improving the electrocata? lytic reduction dechlorination efficiency. Electrolyses of 2 mM 4-CP showed that for the material catalyzed by the Pd/ NiP nanoparticles(1.02 mg),87.5% of 4-CP could be completely dechlorinated within 360 min with an apparent rate constant of 0.0057 min-1,demonstrating an excellent dechlorination performance and high stability of the devel? oped material. This work provides a facile strategy for the synthesis of phosphorus-doped bimetallic nanoparticles, which provides an excellent catalyst and an important reference for the future electrocatalytic dechlorination works.

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黄彬彬 ,秦仕忆 ,曹兴凯 ,.掺磷PdNi催化剂的合成及其电催化脱氯机理研究[J].湖南大学学报:自然科学版,2022,49(6):152~161

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  • 在线发布日期: 2022-06-23
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