posted on 2023-09-25, 17:08authored byTieyue Qi, Shuo Zhang, Tong Li, Lei Xing, Shanlong An, Qiangwei Li, Lidong Wang
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 (Co0) 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
(·SO5– and ·O2–) for the sulfite oxidation on the Co0 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·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.