Yiping Guo,Wei Xie,He Li,Jianping Li,Jun Hu,Honglai Liu
The adsorption desulfurization (ADS) is a promising technology for deep removing thiophene-type sulfurs, yet it remains challenges in maintaining good performance for real applications in the presence of water. Guided by theoretical calculations, we constructed hydrophobic selective channels by crosslinking porous aromatic framework (PAF) of PAF-56 on the surface of adsorbent MOF-199 with Cu nodes reduced. The optimized Cu(I)-BTC@PAF30 shows a high saturated dibenzothiophenes (DBT) adsorption capacity of 61.7 mgS g −1 from the dehydrated model oil. Attributed to the good DBT-affinity (with binding energy (BE) of −90.52 KJ mol −1 ) and water-repulsion (with BE of −14.72 KJ mol −1 ), PAF-56 coating layer significantly improves the hydrophobicity , and keeps the DBT adsorption capacity as high as 50.8 mgS g −1 in the presence of 0.5% (v/v) water, the decline of 17.6% was much smaller than the dramatical 70.9% decrease in pristine Cu(I)-BTC. More importantly, it effectively prevents Cu(I) nodes from the oxidation , and exhibits a superior stable cyclic performance with the removal efficiency above 91% after 20 cycles. Therefore, Cu(I)-BTC@PAF30 can be a good representative of this surface modification strategy to achieve promising application in industrial ADS.
Direct hydrogenation of CO2 to ethanol is a highly economical carbon reduction strategy. However, the CO2 hydrogenation process traditionally requires high temperatures, typically higher than 300 °C, to activate CO2 molecules, which is unfavorable to the formation of ethanol. In contrast, we applied the novel non-thermal plasma to activate CO2 at ambient conditions and a Cu(I)-MOF catalyst to selectively synthesize ethanol for the selective transformation of CO2 into ethanol. The best catalyst, Cu(I)-HKUST-17.5, achieved 41.2% CO2 conversion and up to 62.9% ethanol selectivity under ambient conditions. The control experiments indicated that the Cu(I) sites are key to realizing C–C coupling and ethanol synthesis. An unreported synergistic catalytic mechanism between non thermal plasma and the Cu(I) and Cu(II) sites on the catalyst is proposed based on the DRIFTS analysis. Overall, our work confirms the feasibility of utilizing non thermal plasma assisted catalysis for the selective conversion of CO2 to ethanol under mild conditions.
Shixiang Rao,Hao Jiang,Zheng Li,Guoqing Wang,Shixing Han,Chunguang Li
Marine biofouling poses serious safety risks to offshore infrastructures and leads to substantial economic losses. Although hydrogels have shown significant promise in marine antifouling applications, developing antifouling hydrogels that simultaneously possess excellent mechanical strength and strong antifouling efficiency remains a major challenge. Herein, a high-performance antifouling hydrogel was constructed by incorporating hollow glass microspheres functionalized with a Cu(I) based metal-organic framework (Cu(I)-MOFs) into a poly(vinyl alcohol)/poly(sulfobetaine methacrylate) (PVA/PSBMA) double-network matrix. The as-developed Cu(I)-MOFs/hydrogel composite integrates excellent antifouling and mechanical properties, achieving protein and algal resistance of 99.8% and 99.9%, respectively, as well as a high antibacterial rate of 99.6%. Importantly, the composite reaches a compressive strength of 5.35 MPa, outperforming many existing antifouling hydrogels, and demonstrates low swelling with reliable performance in seawater. In a 100-day field test in a real marine environment, the fouling coverage of as-prepared hydrogel was as low as 0.12%. This work offers an effective and feasible strategy for preventing marine biofouling and also pioneers a new approach for hydrogel applications. Download: Download high-res image (395KB) Download: Download full-size image
The combustion of thiophene sulfides in fuel leads to the release of sulfur oxides (SO x ), which pose significant threats to both ecological systems and human health. Adsorption desulfurization has gained considerable attention from researchers due to its mild operating conditions, low production costs, and minimal impact on octane number. This study investigates the use of Cu-BTC as a platform for developing a novel adsorbent aimed at efficiently removing thiophenic compounds from fuel. Aluminum atoms were incorporated into the framework of Cu-BTC to create micro/mesoporous Al/Cu-BTC. Subsequently, the π-complexation adsorbent Al/Cu(I)-BTC, featuring Lewis acid sites, was synthesized through the in-situ reduction of Al/Cu-BTC using sodium thiosulfate. The adsorption properties of Al/Cu(I)-BTC for thiophene were assessed through both batch and breakthrough experiments. Al/Cu(I)-BTC-0.10(0.28) demonstrated exceptional adsorption performance. The static and dynamic adsorption capacities of thiophene at 500 and 200 ppm were 18.54 mg S/g and 9.49 mg S/g, respectively. Importantly, the adsorption capacity of Al/Cu(I)-BTC-0.10 (0.28) for thiophene in fuel containing 500 ppm sulfur remained at 15.45 mg S/g after six regeneration cycles. In the competitive adsorption of toluene, the adsorption capacity of the adsorbent for thiophene in the fuel containing 200 ppm sulfur was 7.84 mg S/g.
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