N2O 在 ZIF-67 衍生的 Co/CoOx@Carbon 催化剂上的分解和 SO2 干扰,Energy & Fuels

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N2O 在 ZIF-67 衍生的 Co/CoOx@Carbon 催化剂上的分解和 SO2 干扰
Energy & Fuels ( IF 5.2 ) Pub Date : 2021-11-08 , DOI: 10.1021/acs.energyfuels.1c03023
Hairong Tang ₁ , Yong He ₁ , Peixi Liu ₁ , Jiaming Shao _{1,

2} , Fawei Lin ₃ , Zhihua Wang ₁

Affiliation

在无机溶液中以三乙胺作为N ₂ O 分解的去质子化剂合成沸石-咪唑酯骨架前驱体（ZIF-67），并研究了热解产物在不同条件下的催化活性。其中，Co/CoO _x @carbon 催化剂在 N ₂气氛（Co-650N）中在 650 °C 下热解表现出优异的低温催化活性和稳定性，在 305 °C 下分解效率达到 50%，在400 °C，这得益于其大的比表面积、出色的还原性能、丰富的钴活性位点和表面氧物种。此外，利用程序升温脱附 (TPD) 和原位漫反射红外傅里叶变换光谱 (DRIFTS) 结果表明，N ₂ O 分子优先与结合在钴位点上的氧物质结合。吸收的 N ₂ O 分解为 N ₂和氧物种，后者随后转移到碳骨架上。有趣的是，无定形石墨碳骨架在转移/储存活性氧和再生钴位点方面发挥了重要作用。此外，Co-650N对SO ₂表现出更好的抵抗力，效率可以通过加热恢复，最终稳定在100%。最后，Co/CoO _x上N ₂ O 分解和硫中毒-再活化的机制首次提出@carbon 催化剂。

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Decomposition of N2O on ZIF-67-Derived Co/CoOx@Carbon Catalysts and SO2 Interference

Zeolitic-imidazolate framework precursors (ZIF-67) were synthesized in an inorganic solution with triethylamine as a deprotonating agent for N₂O decomposition, and the catalytic activities of the pyrolysis products under different conditions were investigated. Among them, the Co/CoO_x@carbon catalyst pyrolyzed at 650 °C in a N₂ atmosphere (Co-650N) exhibited excellent low-temperature catalytic activity and stability, achieving 50% decomposition efficiency at 305 °C and ∼100% at 400 °C, which benefitted from its large specific surface area, great reduction performance, abundant cobalt active sites, and surface oxygen species. Further, utilizing temperature-programmed desorption (TPD) and in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results, it was found that N₂O molecules preferentially combined with oxygen species bound to cobalt sites. The absorbed N₂O was decomposed into N₂ and oxygen species, and the latter was subsequently transferred to carbon frameworks. Interestingly, the amorphous graphitic carbon frameworks played an important role in transferring/storing active oxygen and regenerating cobalt sites. Moreover, Co-650N exhibited better resistance to SO₂, and the efficiency could be recovered via heating and finally stabilized at 100%. Finally, the mechanisms of N₂O decomposition and sulfur poisoning-reactivation on Co/CoO_x@carbon catalysts were proposed for the first time.

更新日期：2021-11-18

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