Orchestrating dual adsorption sites and unravelling Ce-Mn interaction and reaction mechanisms for efficient NH3-SCR

Zhang, Tiantian; Shi, Tong; Wang, Yan; Hao, Yanheng; Gao, Yonghui; Li, Haorun; Jia, Lin; Liu, Fenrong; Zeng, Shanghong

doi:10.1016/j.jcat.2023.115260

Cited by 15 publications

(1 citation statement)

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“…The high-resolution O 1s XPS spectrum of TCPP exhibited two peaks centered at 531.98 and 533.53 eV, assigned to the CO and C–O bonds in TCPP (Figure c). , Surprisingly, there is a peak centered at 529.44 eV attributed to the Ce–O bond in Figure c, meaning that the Ce 4+ /Ce 3+ ions can form Ce-oxo clusters via coordination with carboxylate ions. As shown in Figure d, the peaks at 882.41, 887.45, 898.58, 900.71, 907.01, and 916.71 eV corresponded to Ce 3d5/2 and Ce 3d3/2 of Ce 4+ in the CMF-200, and the peaks at 885.76 and 904.32 eV corresponded to Ce 3d5/2 and Ce 3d3/2 of Ce 3+ in the CMF-200 sample. − The generation of Ce 3+ ions is mainly attributed to the reduction of Ce 4+ by DMF or dimethylamine at a relatively high reaction temperature. In Figure e, three peaks at 397.66, 399.82, and 400.91 eV could be identified as CN, N–H, and C–N bonds in TCPP, respectively .…”

Section: Resultsmentioning

confidence: 93%

Improving the Photoactivity of Porphyrin-Based Metal–Organic Frameworks via Constructing [Ce–O] Active Site and Vacancy

Cheng,

Ren,

Wang

et al. 2024

Inorg. Chem.

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Defect engineering of metal−organic frameworks (MOFs) is a versatile approach to tailoring their electronic structures and photocatalytic performance. Herein, Ce-based porphyrin MOFs (CMFs) featuring controlled structural defects were successfully prepared using a simple acid modulation strategy to drive the photocatalytic H 2 generation. The [Ce−O] unit serves as the active site via a ligand-to-metal charge transfer process, which has been confirmed by in situ XPS analysis. Abundant exposed coordinatively unsaturated Ce−O centers are beneficial for the adsorption and activation of water molecules, which is an important factor for improving the photocatalytic performance of the synthesized defective MOFs. In addition, optical and electrochemical experiments indicate that CMFs with more oxygen vacancies possess higher charge separation efficiency. As a result, the optimized CMF(Zn)-200 sample afforded high stability and activity in the H 2 generation (up to 1603.3 μmol•g −1 •h −1 under cocatalyst-free conditions) and tetracycline hydrochloride removal efficiency (97%), which was 8.45 and 97 times higher than that of pure meso-tetra(4-carboxyphenyl)porphine. This study demonstrates that effective structural modulation and defect introduction can improve the activity and stability of PMOF-based photocatalysts.

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