scholarly journals Metal–Organic Layers Hierarchically Integrate Three Synergistic Active Sites for Tandem Catalysis

Author(s):  
Yangjian Quan ◽  
Guangxu Lan ◽  
Wenjie Shi ◽  
Ziwan Xu ◽  
Yingjie Fan ◽  
...  
2020 ◽  
Author(s):  
Yangjian Quan ◽  
Guangxu Lan ◽  
Wenjie Shi ◽  
Ziwan Xu ◽  
Yingjie Fan ◽  
...  

2020 ◽  
Author(s):  
Jia-Wei Wang ◽  
Li-Zhen Qiao ◽  
Haodong Nie ◽  
Hai-Hua Huang ◽  
Yi Li ◽  
...  

Abstract Metal-organic layers (MOLs) with ordered structure and molecular tunability are of great potential as heterogeneous catalysts due to their readily accessible active sites. Herein, we demonstrate a facile template strategy to prepare MOLs with a uniform thickness of three metal coordination layers (ca. 1.5 nm) with graphene oxide (GO) as both template and electron mediator. The resulting MOL@GO exhibits an outstanding performance for CO2 photoreduction with a record-high total CO yield of 3133 mmol/gMOL among all the metal-organic framework and MOL catalysts (CO selectivity of 95%). This performance is ca. 34 times higher than that of bulky Co-MOF, [CoL(H2O)2]•0.5H2O (H2L = 5-(1H-1,2,4-triazol-1-yl)isophthalic acid). Systematic studies reveal that well exposed active sites in MOLs, and facile electron transfer between heterogeneous and homogeneous components mediated by GO, greatly contribute to its high activity. This work highlights a facile way for constructing ultrathin MOLs and demonstrate charge transfer pathway between conductive template and catalyst for boosting photocatalysis.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Jia-Wei Wang ◽  
Li-Zhen Qiao ◽  
Hao-Dong Nie ◽  
Hai-Hua Huang ◽  
Yi Li ◽  
...  

AbstractMetal-organic layers with ordered structure and molecular tunability are of great potential as heterogeneous catalysts due to their readily accessible active sites. Herein, we demonstrate a facile template strategy to prepare metal-organic layers with a uniform thickness of three metal coordination layers (ca. 1.5 nm) with graphene oxide as both template and electron mediator. The resulting hybrid catalyst exhibits an excellent performance for CO2 photoreduction with a total CO yield of 3133 mmol g–1MOL (CO selectivity of 95%), ca. 34 times higher than that of bulky Co-based metal-organic framework. Systematic studies reveal that well-exposed active sites in metal-organic layers, and facile electron transfer between heterogeneous and homogeneous components mediated by graphene oxide, greatly contribute to its high activity. This work highlights a facile way for constructing ultrathin metal-organic layers and demonstrates charge transfer pathway between conductive template and catalyst for boosting photocatalysis.


2021 ◽  
Author(s):  
Bahareh ameri ◽  
Akbar Mohammadi Zardkhoshoui ◽  
Saied Saeed Hosseiny Davarani

Metal-organic frameworks (MOFs) derived nanoarchitectures have special features, such as high surface area (SA), abundant active sites, exclusive porous networks, and remarkable supercapacitive performance when compared to traditional nanoarchitectures. Herein,...


Chemosensors ◽  
2021 ◽  
Vol 9 (6) ◽  
pp. 140
Author(s):  
Jing Li ◽  
Keying Xu ◽  
Yang Chen ◽  
Jie Zhao ◽  
Peiyao Du ◽  
...  

Dopamine (DA) is an important catecholamine neurotransmitter that plays a highly relevant role in regulating the central nervous system, and abnormal DA content can cause many immune-related diseases. Hence, it is of significance to sensitively and specifically identify DA for clinical medicine. In this work, Pt/NH2-MIL-101 hybrid nanozymes with bimetallic catalytic centers were fabricated by forming coordinate bonds between Pt nanoparticles (Pt NPs) and –NH2 on metal–organic frameworks (MOF). The catalytic activity of Pt/NH2-MIL-101 was increased by 1.5 times via enlarging the exposure of more active sites and improving the activity of the active sites through the strategy of forming bimetallic catalytic centers. In the presence of DA, competing with 3, 3′, 5, 5′-tetramethylbenzidine (TMB) for the generated hydroxyl radicals (•OH), the blue oxidation state TMB (Ox-TMB) is reduced to colorless TMB, showing dramatic color changes. The Pt/NH2-MIL-101-based colorimetric assay enables the sensitive and robust detection of DA molecules with a detection limit of only 0.42 μM and has an observable potential in clinical applications.


CrystEngComm ◽  
2021 ◽  
Author(s):  
Qing Luo ◽  
Zhen Ding ◽  
Huamin Sun ◽  
Zhen Cheng ◽  
Naien SHI ◽  
...  

Ultrathin two-dimensional (2D) metal-organic framework (MOF) nanosheets are prosperous advanced materials due to their particularly thin thickness and exposed active sites. The difficulty in the controlled synthesis of 2D MOF...


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Gang Zhou ◽  
Peifang Wang ◽  
Hao Li ◽  
Bin Hu ◽  
Yan Sun ◽  
...  

AbstractOxygen evolution reaction (OER) plays a determining role in electrochemical energy conversion devices, but challenges remain due to the lack of effective low-cost electrocatalysts and insufficient understanding about sluggish reaction kinetics. Distinguish from complex nano-structuring, this work focuses on the spin-related charge transfer and orbital interaction between catalysts and intermediates to accelerate catalytic reaction kinetics. Herein, we propose a simple magnetic-stimulation approach to rearrange spin electron occupation in noble-metal-free metal-organic frameworks (MOFs) with a feature of thermal-differentiated superlattice, in which the localized magnetic heating in periodic spatial distribution makes the spin flip occur at particular active sites, demonstrating a spin-dependent reaction pathway. As a result, the spin-rearranged Co0.8Mn0.2 MOF displays mass activities of 3514.7 A gmetal−1 with an overpotential of ~0.27 V, which is 21.1 times that of pristine MOF. Our findings provide a new paradigm for designing spin electrocatalysis and steering reaction kinetics.


Author(s):  
Danni Zhou ◽  
Xinyuan Li ◽  
Huishan Shang ◽  
Fengjuan Qin ◽  
Wenxing Chen

Metal-organic framework (MOF) derived single-atom catalysts (SACs), featured unique active sites and adjustable topological structures, exhibit high electrocatalytic performance on carbon dioxide reduction reactions (CO2RR). By modulating elements and atomic...


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