室温催化湿式氧化处理甲醛废水的Pt/层状双金属氧化物催化剂  

Pt/layered bimetallic oxide catalyst for catalytic wet air oxidation of formaldehyde wastewater at room temperature

作　　者：陈煌斌 刘宁 张诺伟[1] 陈秉辉[1] CHEN Huangbin;LIU Ning;ZHANG Nuowei;CHEN Binghui(National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China)

机构地区：[1]厦门大学化学化工学院,醇醚酯化工清洁生产国家工程实验室,福建厦门361005

出　　处：《厦门大学学报（自然科学版）》2023年第5期758-765,共8页Journal of Xiamen University：Natural Science

基　　金：国家自然科学基金(22272137)。

摘　　要：详细研究了层状双金属氧化物(LDO)制备方法对Pt/LDO催化剂进行催化湿式氧化(CWAO)处理甲醛废水性能的影响,并对制备的催化剂进行X射线衍射、透射电镜、N_(2)物理吸-脱附、H_(2)程序升温还原和X射线光电子能谱等表征.催化剂评价结果表明:在室温和低Pt负载量(质量分数0.25%)的条件下,与Pt/LDO(P)(共沉淀法制备的LDO)相比,Pt/LDO(H)(水热法制备的LDO)催化剂具有更为优异的CWAO处理甲醛废水的催化性能.在室温(30℃)下反应5 h,Pt/LDO(H)可将甲醛完全转化,且能将84.1%的甲醛完全氧化为CO_(2);而在相同条件下,Pt/LDO(P)只能转化63.8%的甲醛,且仅有57.9%的甲醛被完全氧化为CO_(2).Pt/LDO(H)催化剂还具有良好的稳定性,在连续测试的5次反应内,保持高的甲醛转化率(约100%)和总有机碳转化率(约83%).表征结果显示,Pt/LDO(H)催化剂具有高的Pt分散性、强的金属-载体电子相互作用、丰富的表面氧物种、强的氧化能力和良好的抗流失性能,这是其具有优良催化性能的主要原因.In this paper,a thorough study was conducted to evaluate the effect of preparation methods of layered bimetallic oxides(LDO)on the catalytic performance of Pt/LDO for catalytic wet air oxidation(CWAO)of formaldehyde.The prepared catalysts were characterized by X-ray diffraction(XRD),transmission electron microscope(TEM),N_(2)physical adsorption-desorption,H_(2)temperature programmed reduction(H_(2)-TPR)and X-ray photoelectron spectroscopy(XPS).Results of the catalyst evaluation indicate that the Pt/LDO(H)(LDO was prepared by hydrothermal method)exhibits much better catalytic performance than Pt/LDO(P)(LDO was prepared by co-precipitation method)under conditions of room temperature and low Pt loading(0.25%by mass).At room temperature(30℃),Pt/LDO(H)can completely convert HCHO,with 84.1%of HCHO being oxidized to CO_(2)after 5 h of reaction.In contrast,Pt/LDO(P)converts only 63.8%of HCHO and only 57.9%of HCOH is oxidized to CO_(2)under the same reaction condition.Pt/LDO(H)also possesses a good stability.The high HCHO conversion(about 100%)and TOC conversion(83%)is maintained in 5 consecutive runs.The characterization results indicate that the better Pt dispersion,the stronger interaction between metal and carrier,the richer active surface oxygen species,the higher oxidizing ability and the better ability against leaching are attributed to the excellent catalytic property of Pt/LDO(H).

关 键 词：催化湿式氧化 甲醛废水 Pt/层状双金属氧化物催化剂 电子传递 

分 类 号：TQ032[化学工程]