Cabello A, Abad A, Mendiara T, de Las Obras Loscertales M, de Diego L F
Department of Energy and Environment, Instituto de Carboquímica (ICB-CSIC), Miguel Luesma Castán 4, Zaragoza 50018, Spain.
Energy Fuels. 2023 Aug 29;37(18):14254-14267. doi: 10.1021/acs.energyfuels.3c02391. eCollection 2023 Sep 21.
In the present study, the performance of a CaMnTiMgO perovskite used as an oxygen carrier to burn sour gas with different HS concentrations (up to 3000 vppm) in a continuous 500 W chemical looping combustion (CLC) prototype was investigated. After 29 h of sour gas combustion, the combustion efficiency had dropped by 18% in comparison with the reference test without sulfur addition. The characterization of the used particles of the perovskite confirmed that the presence of sulfur in the fuel gas had a poisonous effect through the formation of undesired compounds, such as CaSO. The reactivity with CH and oxygen uncoupling capacity decreased, which could explain the decrease in the combustion efficiency. Two regeneration processes, one at high temperature (1273 K) and another one at low temperature (773-873 K), were carried out in a batch fluidized bed reactor to remove the amount of sulfur accumulated in the oxygen carrier particles. The detection of appreciable amounts of gaseous sulfur-based compounds (SO and HS) during the experimentation and the postcharacterization results obtained through different techniques such as X-ray diffraction, ultimate analysis, and thermogravimetric analysis confirmed the effectiveness of both processes. Finally, the feasibility of implementation of the regeneration processes in a commercial CLC unit was thoroughly analyzed.
在本研究中，对一种用作氧载体的钙锰钛镁氧化物钙钛矿在连续500瓦化学链燃烧（CLC）原型装置中燃烧不同硫化氢浓度（高达3000体积百万分率）酸性气体的性能进行了研究。在燃烧酸性气体29小时后，与不添加硫的参考试验相比，燃烧效率下降了18%。对用过的钙钛矿颗粒进行表征证实，燃料气中硫的存在通过形成不期望的化合物（如硫酸钙）产生了毒害作用。与甲烷的反应性和氧解耦能力降低，这可以解释燃烧效率的下降。在间歇流化床反应器中进行了两个再生过程，一个在高温（1273K）下进行，另一个在低温（773 - 873K）下进行，以去除氧载体颗粒中积累的硫量。实验过程中检测到大量气态硫基化合物（二氧化硫和硫化氢），并且通过不同技术（如X射线衍射、元素分析和热重分析）获得的表征后结果证实了这两个过程的有效性。最后，对在商业CLC装置中实施再生过程的可行性进行了全面分析。
