Desulfurization technology is rather difficult and urgently needed for carbon dioxide(CO_(2))utilization in industry.A new Cu(I)-based adsorbent was synthesized and examined for the capacity of removing carbonyl sulfi...Desulfurization technology is rather difficult and urgently needed for carbon dioxide(CO_(2))utilization in industry.A new Cu(I)-based adsorbent was synthesized and examined for the capacity of removing carbonyl sulfide(COS)from a CO_(2)stream in an effort to solve the competitive adsorption between CO_(2)and COS and to seek opportunity to advance adsorption capacity.A wide range of character-ization techniques were used to investigate the physicochemical properties of the synthesized Cu(I)adsorbent featuringπ-complexation and their correlations with the adsorption performance.Meanwhile,the first principal calculation software CP2K was used to develop an understanding of the adsorption mechanism,which can offer useful guidance for the adsorbent regeneration.The synthesized Cu(I)adsorbent,prepared by using copper citrate and citric acid on the ZSM-5(SiO_(2)/Al_(2)O_(3)=25)carrier,outperformed other adsorbents with varying formulations and carriers in adsorption capacities.Through optimization of the preparation and adsorption conditions for various adsorbents,the breakthrough adsorption capacity(Qb)for COS was further enhanced from 2.19 mg/g to 15.36 mg/g.The formed stableπ-complex bonds between COS and Cu(I),as confirmed by density func-tional theory calculations,were verified by the significant improvement in the adsorption capacity after regeneration at 600°C.The above advantages render the novel synthesized Cu(I)adsorbent a promising candidate featuring cost-effectiveness,high efficacy and good regenerability for desulfurization from a CO_(2)stream.展开更多
基金supported by the National Key Research and Development Program of China(2022YFA1504402)National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC)+2 种基金the National Natural Science Foundation of China(22472016 and U23B20169)Key R&D Program of Ningbo(No.2023Z144)the Fundamental Research Funds for the Central Universities(DUT22LAB601).
文摘Desulfurization technology is rather difficult and urgently needed for carbon dioxide(CO_(2))utilization in industry.A new Cu(I)-based adsorbent was synthesized and examined for the capacity of removing carbonyl sulfide(COS)from a CO_(2)stream in an effort to solve the competitive adsorption between CO_(2)and COS and to seek opportunity to advance adsorption capacity.A wide range of character-ization techniques were used to investigate the physicochemical properties of the synthesized Cu(I)adsorbent featuringπ-complexation and their correlations with the adsorption performance.Meanwhile,the first principal calculation software CP2K was used to develop an understanding of the adsorption mechanism,which can offer useful guidance for the adsorbent regeneration.The synthesized Cu(I)adsorbent,prepared by using copper citrate and citric acid on the ZSM-5(SiO_(2)/Al_(2)O_(3)=25)carrier,outperformed other adsorbents with varying formulations and carriers in adsorption capacities.Through optimization of the preparation and adsorption conditions for various adsorbents,the breakthrough adsorption capacity(Qb)for COS was further enhanced from 2.19 mg/g to 15.36 mg/g.The formed stableπ-complex bonds between COS and Cu(I),as confirmed by density func-tional theory calculations,were verified by the significant improvement in the adsorption capacity after regeneration at 600°C.The above advantages render the novel synthesized Cu(I)adsorbent a promising candidate featuring cost-effectiveness,high efficacy and good regenerability for desulfurization from a CO_(2)stream.
