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氟和磷在以磷石膏为载氧体的化学链气化中的化学行为。

Chemical behavior of fluorine and phosphorus in chemical looping gasification using phosphogypsum as an oxygen carrier.

机构信息

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, Yunnan, 650093, China.

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, Yunnan, 650093, China.

出版信息

Chemosphere. 2020 Jun;248:125979. doi: 10.1016/j.chemosphere.2020.125979. Epub 2020 Jan 22.

DOI:10.1016/j.chemosphere.2020.125979
PMID:32028158
Abstract

In China, the amount of phosphogypsum (PG) has exceeded 250 million tons with more than 55 million tons of growth rates each year. As the micro constituent, fluorine and phosphorus restrict the resourceful disposal of PG. This paper focused on chemical looping gasification (CLG) which used PG as an oxygen carrier, systematically investigated the gasification performance and chemical behavior of fluorine and phosphorus contained in PG during CLG process. Main conclusions are as follows. The main pollutant of chemical looping gasification process was HF, which was transformed from NaF. Phosphorus transformed from water-soluble phosphorus (Ca(HPO), Ca(HPO)) into insoluble Ca(PO).20 reducing-oxidizing cycles were investigated, and a less and less fluorine content in oxygen carrier was found because its phase transformation from solid NaF to gaseous HF, and the phosphorus content in oxygen carrier changed slightly under the current conditions. The Ca(PO) particle layers existed in both the middle of the reduced solid particles and the middle of the cycled oxygen carrier particles, confirmed to actually act as a glue between the particles. Furthermore, transformation routes of fluorine and phosphorus during the CLG process were discussed and the generation of syngas in CLG process needed to be purified.

摘要

在中国,磷石膏(PG)的储量已经超过 2.5 亿吨,每年还以超过 5500 万吨的速度增长。作为微观成分,氟和磷限制了 PG 的资源化处理。本文聚焦于化学链气化(CLG),将 PG 用作载氧体,系统研究了 PG 在 CLG 过程中含氟和含磷的气化性能和化学行为。主要结论如下。化学链气化过程的主要污染物是 HF,它是由 NaF 转化而来的。磷从水溶性磷(Ca(HPO)4、Ca(HPO)3)转化为不溶性 Ca(PO)4。进行了 20 次还原-氧化循环实验,发现载氧体中的氟含量越来越少,因为它从固相 NaF 向气相 HF 的相转变,并且在当前条件下,载氧体中的磷含量变化不大。在还原的固体颗粒中间和循环的载氧体颗粒中间都存在 Ca(PO)4 颗粒层,证实了它们实际上起到了颗粒之间的粘结作用。此外,还讨论了 CLG 过程中氟和磷的转化途径,需要对 CLG 过程中产生的合成气进行净化。

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