Synthesis of (100) surface oriented MIL-88A-Fe with rod-like structure and its enhanced fenton-like performance for phenol removal
Synthesis of (100) surface oriented MIL-88A-Fe with rod-like structure and its enhanced fenton-like performance for phenol removal
复制标题
具有棒状结构的(100)表面取向MIL-88A-Fe的合成及其增强的类芬顿去除苯酚性能
DOI：
10.1016/j.apcatb.2019.118064
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发表时间：
2019-12-15
影响因子：
22.1
通讯作者：
Lu, Shuxiang
中科院分区：
文献类型：
--
作者：
Liao, Xiaoyuan;Wang, Fan;Lu, Shuxiang
MIL-88A-Fe的形态对其类Fenton性能有很大影响。在本工作中，通过改变溶剂的比例，制备了棒状、纺锤状和金刚石状的MIL-88A-Fe。通过X射线衍射、扫描电子显微镜、透射电子显微镜、X射线光电子能谱、电子自旋共振和密度泛函计算对其物化性能进行了全面的表征，证实了MIL-88A-Fe的(100)暴露比决定了其催化性能。在MIL-88A-Fe的(100)面上，H_2O_2解离成(OH)-O-中心点的势垒较低(解离能为0.58 eV)，相应的(101)面势垒为0.8 eV。类Fenton性能的顺序为：r-MIL-88A(TOF 5.0h(-1))>；S-MIL-88A(TOF 3.3h(-1))>；D-MIL-88A(TOF 2.5h(-1))，当r-MIL-88A作为催化剂时，在室温条件下，在H_2O_2的帮助下，苯酚在15min内可脱除100%，其活性优于已报道的铁基MOF，如MIL-88B-Fe、MIL-101-Fe、MIL-53(Fe)等，这一发现可能是通过选择合适的铁基金属有机骨架的晶相来提供Fenton类催化剂。
Morphology of MIL-88A-Fe greatly affects their Fenton-like performance. In this work, rod-like, spindle-like and diamond-like MIL-88A-Fe was prepared by changing the ratio of solvents in solvothermal process. Their physicochemical properties are fully investigated by XRD, SEM, TEM, XPS, ESR, and DFT calculation, which confirmed that the exposed (100) ratio of MIL-88A-Fe determined its catalytic performance. The (100) surface of MIL-88A-Fe showed lower energy barrier for H2O2 dissociated into (OH)-O-center dot (dissociated energy 0.58 eV), corresponding value is 0.8 eV for (101) surface. The Fenton-like performance has the order of r-MIL-88A (TOF 5.0 h(-1)) > s-MIL-88A (TOF 3.3 h(-1)) > d-MIL-88A (TOF 2.5 h(-1)), when r-MIL-88A used as catalyst, phenol could be removed 100% in 15 min by the help of H2O2 at room conditions, its activity are better than that of reported Febased MOFs, such as MIL-88B-Fe, MIL-101-Fe, and MIL-53(Fe) etc. This finding probably provide a Fenton-like catalyst by choosing the suitable crystal phase of Fe-based metal organic framework.