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Hg0 removal performance at low temperature by mesoporous MOF-derived Cr2O3 nanoparticle with enriched metal sites and oxygen vacancy: Mechanism study on the role of oxygen species
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-05-10 , DOI: 10.1016/j.cej.2023.143402
Xifeng Zhu , Yuan Liu , Yi Xiao , Longchun Zhong , Tao Wang , Yuguo Wang , Wei-Ping Pan

The oxidation adsorption of Hg0 by metal oxide is an effective method to remove Hg0. A novel high-performance catalyst Cr2O3-MOF was prepared by direct calcination of MIL-101 (Cr) to improve the mercury adsorption capacity of MOFs at lower temperature ranges, overcome the weak resistance to different flue gas components and increase the recycling capacity. Cr2O3-MOF retains the skeleton structure of MOF with small particle sizes and scattered active sites. The oxygen vacancy (OV) formed after calcination can be filled by free oxygen to adjust the catalytic performance of the surface. Thus, Cr2O3-MOF has a mercury removal capacity to be reached at 100% in a wide temperature range (30–200 °C), especially has the ability of mercury adsorption at room temperature that many MOF adsorbents do not have. After continuous adsorption at 30 °C for 50 h, the mercury removal efficiency was maintained at 90.3%, and it could be recycled. Cr2O3-MOF also has excellent resistance to flue gas components such as SO2, NH3, NO, and H2O. Based on different characterization methods and density functional theory (DFT), the transition state theory explains that adsorbed oxygen (OAds) filled in OV has higher mercury capture activity than that of natural lattice oxygen (OLat) in the adsorbent. More importantly, compared with noble metal supported monatomic catalysts, Cr2O3-MOF has a lower cost with higher mercury removal efficiency, it has more industrial application prospects.



中文翻译:

具有富金属位点和氧空位的介孔 MOF 衍生的 Cr2O3 纳米粒子在低温下的 Hg0 去除性能:氧物种作用的机理研究

金属氧化物对Hg 0的氧化吸附是去除Hg 0的有效方法。直接煅烧MIL-101(Cr)制备新型高性能催化剂Cr 2 O 3 -MOF,提高MOFs在较低温度范围内的汞吸附能力,克服对不同烟气成分的弱抵抗力提高回收率容量。Cr 2 O 3 -MOF保留了MOF的骨架结构,粒径小,活性位点分散。煅烧后形成的氧空位(O V )可以被游离氧所填补,从而调节表面的催化性能。因此,Cr 2 O 3-MOF在很宽的温度范围内(30-200℃)具有100%的除汞能力,尤其是具有许多MOF吸附剂所不具备的室温吸附汞的能力。30℃连续吸附50h后,脱汞效率保持在90.3%,可循环使用。Cr 2 O 3 -MOF对SO 2、NH 3、NO和H 2 O等烟气成分也具有优异的抵抗能力。基于不同的表征方法和密度泛函理论(DFT),过渡态理论解释了吸附氧(O Ads ) 填充在 O V中的汞捕获活性高于天然晶格氧 (OLat ) 在吸附剂中。更重要的是,与贵金属负载单原子催化剂相比,Cr 2 O 3 -MOF成本更低,脱汞效率更高,更具工业应用前景。

更新日期:2023-05-10
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