Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 57, Issue 41, Pages 15759-15770Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.3c06258
Keywords
arsenic removal; ammonium sulfite oxidation; lanthanum; catalysis; desulfurization
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This study fabricates nitrogen-doped porous carbon coembedded with lanthanum and cobalt (La-Co@NPC) as a dual-functional catalyst for sulfite oxidation and arsenic removal in the desulfurization process. The La-Co@NPC/S(IV) catalytic system generates strongly oxidizing free radicals for sulfite oxidation and oxidizes As(III) into As(V). The results show high efficiency in ammonium sulfite oxidation and arsenic removal, making it significant for the high-value recovery of sulfur resources in coal-fired desulfurization.
Ammonia desulfurization is a typical resource-recovery-type wet desulfurization process that is widely used in coal-fired industrial boilers. However, the sulfur recovery is limited by the low oxidation rate of byproduct (ammonium sulfite), leading to secondary SO2 pollution due to its easy decomposability. In addition, the high toxic arsenic trace substances coexisting in desulfurization liquids also reduce the quality of the final sulfate product, facing with high environmental toxicity. In this study, nitrogen-doped porous carbon coembedded with lanthanum and cobalt (La-Co@ NPC) was fabricated with heterologous catalytic active sites (Co-0) and adsorption sites (LaOCl) to achieve sulfite oxidation and the efficient removal of high toxic trace arsenic for the recovery of high-value ammonium sulfate from the desulfurization liquid. The La-Co@NPC/S(IV) catalytic system can generate numerous strongly oxidizing free radicals (center dot SO5- and center dot O-2(-)) for the sulfite oxidation on the Co-0 site, as well as oxidative detoxification of As(III) into As(V). Subsequently, arsenic can be removed through chemical adsorption on LaOCl adsorption sites. By using the dual-functional La-Co@NPC at a concentration of 0.25 g/L, the rate of ammonium sulfite oxidation reached 0.107 mmol/L center dot s(-1), the arsenic (1 mg/L) removal efficiency reached 92%, and the maximum adsorption capacity of As reached up to 123 mg/g. This study can give certain guiding significance to the functional material design and the coordinated control of multiple coal-fired pollutants in desulfurization for high-value recovery of sulfur resources.
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