期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 56, 期 7, 页码 4507-4517出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.2c00031
关键词
halloysite nanotubes; arsenic; capture; flue gas; copper chloride
资金
- National Natural Science Foundation of China [22176056]
- National Key R&D Program of China [2018YFB0605101]
- Fundamental Research Funds for the Central Universities [2017ZZD07]
In this study, CuCl2-modified halloysite nanotubes (CuCl2-HNTs) were successfully prepared as an adsorbent for the removal of arsenic from high-temperature coal combustion flue gas. The CuCl2-HNTs showed high arsenic adsorption capacity and tolerance to high concentrations of gases. The captured arsenic could be stable at high temperatures.
Gaseous arsenic emitted from coal combustion flue gas (CCFG) causes not only severe contamination of the environment but also the failure of selective catalytic reduction (SCR) catalysts in power plants. Development of inexpensive and effective adsorbents or techniques for the removal of arsenic from high-temperature CCFG is crucial. In this study, halloysite nanotubes (HNTs) at low price were modified with CuCl2 (CuCl2-HNTs) through ultrasound assistance and applied for capturing As2O3(g) in simulated flue gas (SFG). Experiments on arsenic adsorption performance, adsorption mechanism, and adsorption energy based on density functional theory were performed. Modification with CuCl2 clearly enhanced the arsenic uptake capacity (approximately 12.3 mg/g) at 600 degrees C for SFG. The adsorbent exhibited favorable tolerance to high concentrations of NOx and SOx. The As2O3(III) was oxidized and transformed into As2O3(V) on the CuCl2-HNTs. The Al-O bridge had the highest adsorption energy for the O end of the As-O group (-2.986 eV), and the combination formed between arsenic-containing groups and aluminum was stable. In addition, the captured arsenic could be stabilized in the sorbent at high temperature, making it possible to use the sorbent before the SCR system. This demonstrates that CuCl2-HNTs is a promising sorbent for arsenic oxidation and removal from CCFG.
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