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首页> 外文期刊>ACS Sustainable Chemistry & Engineering >Effect of Humidity on the Sorption of H2S from Multicomponent Acid Gas Streams on Silica-Supported Sterically Hindered and Unhindered Amines
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Effect of Humidity on the Sorption of H2S from Multicomponent Acid Gas Streams on Silica-Supported Sterically Hindered and Unhindered Amines

机译：湿度对二种酸气流的H2S吸附的影响二氧化硅载体的空间阻尼和无阻尼胺

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摘要

The sorption of H2S on a silica-supported sterically hindered secondary amine and a supported unhindered tertiary amine is investigated using fixed bed breakthrough experiments. In situ Fourier transform infrared spectroscopy and computational analysis are used to elucidate the structure of the surface species formed during humid H2S sorption. Additionally, the cyclic stability of the amine-functionalized silica sorbent is assessed using NMR spectroscopy, N-2 physisorption, and elemental analysis. For all sorbents under dry conditions, the physisorption of H2S on the amines led to low H2S sorption capacities, but under humid conditions, a strongly chemisorbed species is formed, which leads to an increase in the H2S sorption capacity. These findings are supported by density functional theory (DFT) calculations, which support the formation of a chemisorbed and stable HS-species in the presence of H2O. As a result of the strongly bound species, the sorbents require humid temperature swing sorptiondesorption cycles for efficient sorbent regeneration under the conditions studied, with temperature swings using dry gas failing to effectively desorb the H2S. For competitive H2S/CO2 sorption under mixed gas conditions (CH4/CO2/H2S/H2O), the selectivity for H2S sorption over CO2 is demonstrated to result from kinetic factors, with reaction barriers playing a major role under humid conditions. Overall, the structure of the silica framework and organic moieties are maintained for both sorbents after extended humid H2S exposure. The results in this work confirm the positive effect of humidity on the H2S sorption capacity of silica-supported sterically hindered and unhindered amines.
机译：使用固定床突破实验研究了二氧化硅支持的空间阻碍的二氧化胺和负载的无阻尼叔胺的H2S对H 2 S的吸附。原位傅里叶变换红外光谱和计算分析用于阐明在潮湿的H2S吸附过程中形成的表面物种的结构。另外，使用NMR光谱，N-2理由和元素分析评估胺官能化二氧化硅吸附剂的环状稳定性。对于干燥条件下的所有吸附剂，H 2 S对胺对的物理吸附能力低，但在潮湿条件下，形成强化学的物种，导致H2S吸附能力的增加。这些发现由密度泛函理论（DFT）计算支持，其在H 2 O存在下支持形成化学和稳定的HS型。由于具有强烈的物种，吸附剂需要潮湿的温度挥索溶解​​循环，以便在所研究的条件下有效吸附剂再生，使用干气体未能有效地解吸H2S。对于混合气体条件下的竞争性H 2 S / CO2吸附（CH4 / CO2 / H2S / H2O），对CO2的H2S吸附的选择性被证明是由动力学因子产生的，反应障碍在潮湿的条件下发挥重要作用。总的来说，在延长潮湿的H2S暴露后，对两种吸附剂保持了二氧化硅框架和有机部分的结构。这项工作的结果证实了湿度对二氧化硅的空间妨碍和无阻尼胺的H2S吸附能力的积极作用。

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