负载型零价过渡金属在双氧化体系下降解高稳定油田污染物  

The degradation of highly stable oilfield pollutants by supported zero-valent transition metals in a dual-oxidation system

作　　者：白兵兵 杨晨晔 豆龙龙 周瑞[1] 张洁[1,2] 汤颖[1,2] BAI Bingbing;YANG Chenye;DOU Longlong;ZHOU Rui;ZHANG Jie;TANG Ying(Shaanxi Province Key Laboratory of Environmental Pollution Control and Reservoir Protection Technology of Oilfields,Xi'an Shiyou University,Xi'an 710065,China;Shaanxi University Engineering Research Center of Oil and Gas Field Chemistry,Xi'an Shiyou University,Xi'an 710065,China;The Tenth Oil Production Plant of Changqing Oilfield Branch,China National Petroleum Corporation,Xi'an 710060,China)

机构地区：[1]西安石油大学陕西省油气田环境污染控制技术与储层保护重点实验室,陕西西安710065 [2]西安石油大学油气田化学陕西省高校工程研究中心,陕西西安710065 [3]中国石油天然气集团公司长庆油田分公司第十采油厂,陕西西安710060

出　　处：《工业水处理》2024年第12期123-130,共8页Industrial Water Treatment

基　　金：陕西省重点研发计划项目(2023-YBGY-052);陕西省教育厅重点科学研究计划项目(21JY035)。

摘　　要：过硫酸盐单一氧化技术在过渡金属活化下可有效降解有机污染物,但存在氧化剂投加量过大、pH适用范围窄和金属离子浸出造成二次污染等问题。为了应对上述问题,采用浸渍还原法将过渡金属Cu负载至水滑石(LDHs)载体上,得到高分散负载型零价铜固体催化剂(Cu^(0)@LDHs)。通过Cu^(0)@LDHs活化过氧化氢-过硫酸钠(H_(2)O_(2)-Na_(2)S_(2)O_(8))双氧化体系降解油田高聚物羟丙基瓜尔胶(HPG)。对反应条件的优化结果表明,在pH为3~11的范围内,H_(2)O_(2)-Na_(2)S_(2)O_(8)双氧化体系对HPG均能保持较高的降解效果,25 min内降解率皆高于76.30%,且120 min后COD去除率最高可达93.91%。Cu^(0)@LDHs循环再生5次后仍能保持良好的催化活性,其对HPG的降解效率能保持在80%以上。在此过程中,·OH和SO_(4)^(·-)是主要活性物种并且二者间存在协同作用。反应前后Cu^(0)@LDHs的XRD、SEM、BET表征结果表明,该催化剂所表现出的高活性主要归结于高度分散在水滑石载体表面的Cu^(0)具有良好的活性以及稳定性。The peroxydisulfate single-oxidation technology can effectively degrade organic pollutants under the activation of transition metals.However,there are issues such as excessive oxidant dosage,narrow pH range,and secondary pollution caused by metal ions leaching.To address these problems,a highly dispersed supported zero-valent copper catalyst(Cu^(0)@LDHs)was obtained by loading transition metal copper onto hydrotalcite(LDHs)carriers by the impregnation-reduction method.Cu^(0)@LDHs was used to activate the hydrogen peroxide-sodium persulfate(H_(2)O_(2)-Na_(2)S_(2)O_(8))dual-oxidation system for the degradation of oilfield hydroxypropyl guar gum(HPG).Based on the optimization of reaction conditions,it was found that within the pH range of 3 to 11,the H_(2)O_(2)-Na_(2)S_(2)O_(8) dual-oxidation system still maintained a high degradation effect on HPG,with degradation rates higher than 76.30% at 25 min,and COD removal rate of 93.91% after 120 min.Cu^(0)@LDHs maintained good catalytic activity even after 5 cycles of regeneration,with HPG degradation efficiency of above 80%.During this process,·OH and SO_(4)^(·-)were identified as the main active species,and there was a synergistic effect between them.XRD,SEM,and BET characterization of Cu^(0)@LDHs before and after the reaction indicated that the high activity of the catalyst was mainly attributed to the highly dispersed Cu^(0) on the surface of the hydrotalcite carrier,which exhibited excellent activity and stability.

关 键 词：过氧化氢-过硫酸钠 双氧化体系 羟丙基瓜尔胶 负载型零价金属催化剂 

分 类 号：X741[环境科学与工程—环境工程]