微波辅助合成镁铝类水滑石基氧化物及其在含O2/H2S气氛下的COS水解催化行为OA
Microwave-assisted synthesis of MgAl hydrotalcite-based oxides and their catalytic performance for COS hydrolysis under atmosphere containing O2/H2S
COS水解催化在工业气净化脱硫中具有重要意义.镁铝类水滑石基氧化物(MgAl-MMO)在简单气氛(COS+H2O)下可有效催化COS水解,然而O2/H2S对MgAl-MMO的催化影响作用尚不明晰,同时现有催化剂合成方法耗时较长.探索了微波辅助合成MgAl-MMO的可行性,并研究了其在反应气含O2/H2S下的催化行为.结果表明,80℃微波晶化及n(Mg)/n(Al)=2时所制催化剂COS水解性能最佳,其在反应气含1.0%(体积分数)O2气氛中,COS转化率及H2S选择性均为100.0%并保持540 min;但O2体积分数增大至1.5%时,COS转化率及H2S选择性明显降低(分别下降63.2%与68.8%),主要归因于高O2体积分数下H2S催化氧化导致催化剂表面硫沉积加剧;无O2环境中H2S在催化过程中导致催化剂中毒,且中毒程度随H2S质量浓度增大而加剧:含198 mg/m3 H2S下COS转化率和H2S选择性在100 min时分别降至37.4%和5.3%;1.0%O2与198 mg/m3 H2S共存进一步加快催化剂失活,加剧了表面硫酸盐化及中弱碱相对含量减小,且H2S对催化剂的不利影响显著大于O2,反应85 min时COS转化率与H2S选择性分别仅为20.2%、1.4%.
COS hydrolysis catalysis is important in industrial gas purification and desulfurization.MgAl hydrotalcite-based oxides(MgAl-MMO)can effectively catalyze COS hydrolysis in a simple atmosphere(COS+H2O).However,the catalytic effect of O2/H2S on MgAl-MMO is not clear,and the existing synthesis methods are time-consuming.The feasibility of microwave-assisted synthesis of MgAl-MMO was explored and its catalytic behavior under reaction gas containing O2/H2S was investigated.The results show that the best performance of the catalyst for COS hydrolysis is achieved by microwave crystallization at 80℃and n(Mg)/n(Al)of 2.The COS conversion rate and H2S selectivity of the catalysts are 100.0%and maintain for 540 min in in the reaction gas(O2 volume fraction of 1.0%).However,the COS conversion rate and H2S selectivity decrease significantly(by 63.2%and 68.8%,respectively)when the O2 volume fraction increases to 1.5%,which is mainly attributed to the increase of sulfur deposition on the catalyst surface due to the catalytic oxidation of H2S at high O2 volume fraction.H2S in the O2-free environment leads to catalyst poisoning during the catalytic process,and the degree of poisoning increases with the increase of H2S mass concentration:COS conversion rate and H2S selectivity with 198 mg/m3 H2S decrease to 37.4%and 5.3%after 100 mintutes,respectively.The coexistence of 1.0%O2 and 198 mg/m3 H2S further accelerate the catalyst deactivation,exacerbate the surface sulfation and the relative content of medium bases and weak bases decreased significantly,and the detrimental effect of H2S on the catalyst is significantly greater than that of O2,with the COS conversion rate and the H2S selectivity of only 20.2%and 1.4%,respectively,after 85 minutes of reaction.
吴俊宏;段新伟;杨敏;米杰;王建成;武蒙蒙
太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室,山西 太原 030024太原理工大学 煤科学与技术教育部重点实验室,山西 太原 030024太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室,山西 太原 030024太原理工大学 煤科学与技术教育部重点实验室,山西 太原 030024太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室,山西 太原 030024太原理工大学 煤科学与技术教育部重点实验室,山西 太原 030024
化学化工
微波合成镁铝类水滑石基氧化物COS水解H2S失活
microwave synthesisMgAl hydrotalcite-based oxidesCOS hydrolysisH2Sdeactivation
《低碳化学与化工》 2026 (1)
98-107,10
国家自然科学基金面上项目(22278294)山西省自然科学基金面上项目(20210302123191).
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