Chen Xiaoyu, Feng Xuan, Xie Yibing, Wang Langlang, Chen Lu, Wang Xueqian, Ma Yixing, Ning Ping, Pu Yu
Zhejiang Nanhua Anti-corrosion Equipment Co., LTD., Hangzhou 311255, China.
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, No. 727, Jingming South Road, Chenggong New District, Kunming 650500, China.
ACS Omega. 2022 May 11;7(20):17358-17368. doi: 10.1021/acsomega.2c01355. eCollection 2022 May 24.
Traditional adsorbents undershot the expectations for arsine (AsH) removal under low-temperature operation conditions in the industry. In this study, the copper (Cu) precursor was used to modify activated carbon and yield novel adsorbents by low-temperature roasting for high-efficiency removal of AsH. The best conditions were determined as impregnation with 2 mol/L Cu(NO) adsorbent and roasting at 180 °C. At a reaction temperature of 40 °C and an oxygen content of 1%, the AsH removal efficiency reached over 90% and lasted for 40 h and the best capacity of 369.6 mg/g was obtained with the Cu/Ac adsorbent. The characterization results showed the decomposition of Cu(NO) during the low-temperature roasting process to form surface functional groups. The formation of the important intermediate Cu(NO)(OH) in the decomposition of Cu(NO) into CuO plays a role in the good regeneration performance of the Cu/Ac adsorbent using water washing and the gas regeneration method. The results of in situ diffuse reflectance infrared Fourier transform spectroscopy combined with X-ray photoelectron spectroscopy demonstrated that the interaction of trace oxygen with Lewis (L) acid sites increased chemisorbed oxygen by 17.34%, significantly promoting the spontaneity of AsH oxidation reaction. These results provide a friendly economic method with industrial processes practical for AsH removal.
传统吸附剂在工业低温运行条件下对砷化氢（AsH）的去除效果未达预期。在本研究中，采用铜（Cu）前驱体对活性炭进行改性，并通过低温焙烧制备新型吸附剂以高效去除AsH。确定最佳条件为用2 mol/L Cu(NO₃)₂浸渍吸附剂并在180 °C下焙烧。在反应温度为40 °C且氧气含量为1%时，Cu/Ac吸附剂对AsH的去除效率达到90%以上并持续40 h，且获得了369.6 mg/g的最佳吸附容量。表征结果表明，Cu(NO₃)₂在低温焙烧过程中分解形成表面官能团。Cu(NO₃)₂分解为CuO过程中重要中间体Cu₂(OH)₃NO₃的形成，对Cu/Ac吸附剂采用水洗和气体再生法具有良好的再生性能起到了作用。原位漫反射红外傅里叶变换光谱结合X射线光电子能谱的结果表明，痕量氧与路易斯（L）酸位点的相互作用使化学吸附氧增加了17.34%，显著促进了AsH氧化反应的自发性。这些结果提供了一种对工业过程友好且经济实用的AsH去除方法。
