One-Step Synthesized SO42–/ZrO2-HZSM-5 Solid Acid Catalyst for Carbamate Decomposition in CO2 Capture,Environmental Science & Technology

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One-Step Synthesized SO42–/ZrO2-HZSM-5 Solid Acid Catalyst for Carbamate Decomposition in CO2 Capture
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-10-15 , DOI: 10.1021/acs.est.0c04946
Lei Xing _{1,

2} , Kexin Wei _{1,

2} , Qiangwei Li _{1,

2} , Rujie Wang _{1,

2} , Shihan Zhang ₃ , Lidong Wang _{1,

2}

Affiliation

Amine-based CO₂ capture technology requires high-energy consumption because the desorption temperature required for carbamate breakdown during absorbent regeneration is higher than 110 °C. In this study, we report a stable solid acid catalyst, namely, SO₄^2–/ZrO₂-HZSM-5 (SZ@H), which has improved Lewis acid sites (LASs) and Bronsted acid sites (BASs). The improved LASs and BASs enabled the CO₂ desorption temperature to be decreased to less than 98 °C. The BASs and LASs of SZ@H preferred to donate or accept protons; thus, the amount and rate of CO₂ desorption from spent monoethanolamine were more than 40 and 37% higher, respectively, when using SZ@H than when not using any catalyst. Consequently, the energy consumption was reduced by approximately 31%. A catalyzed proton-transfer mechanism is proposed for SZ@H-catalyzed CO₂ regeneration through experimental characterization and theoretical calculations. The results reveal the role of proton transfer during CO₂ desorption, which enables the feasibility of catalysts for CO₂ capture in industrial applications.

中文翻译：

一步法合成SO ₄^{2- /}的ZrO ₂在CO -HZSM -5-固体酸催化剂用于氨基甲酸盐分解₂捕获

基于胺的CO ₂捕集技术需要消耗大量的能量，因为吸收剂再生期间氨基甲酸酯分解所需的解吸温度高于110°C。在这项研究中，我们报告了一种稳定的固体酸催化剂，即SO ₄^2- / ZrO ₂ -HZSM-5（SZ @ H），该催化剂具有改善的路易斯酸位点（LASs）和布朗斯台德酸位点（BASs）。改进的LAS和BAS使CO _2的解吸温度降低到低于98°C。SZ @ H的BAS和LAS倾向于捐赠或接受质子；因此，CO ₂的量和速率使用SZ @ H时，用过的单乙醇胺的脱附率分别比不使用任何催化剂时高40％和37％。因此，能耗降低了约31％。通过实验表征和理论计算，提出了SZ @ H催化CO ₂再生的催化质子转移机理。结果揭示了质子转移在CO ₂解吸过程中的作用，这使催化剂在工业应用中捕获CO ₂的可行性成为可能。

更新日期：2020-10-15

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