3d transitional-metal single atom catalysis toward hydrogen evolution reaction on MXenes supports

Shen, Zihan; Fan, Xiaoli; Ma, Shuo; An, Yurong; Yang, Danxi; Guo, Nijing; Luo, Zhifen; Hu, Yan

doi:10.1016/j.ijhydene.2020.03.174

Cited by 72 publications

(36 citation statements)

References 55 publications

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“…There are various binding sites on the surface of Mo 2 CS 2 monolayer, such as a top site on the top of sulphur atoms (Site I), a hollow site formed by three neighboring sulphur (S) atoms with a top layer Mo atom (Site II), and a bottom layer of Mo atom (Site III). We optimized the geometries of Co atom binding at the three surface sites and found that the Co single atom prefered to locate at the most stable site on the top of the Mo atom (Site II), consistent with previous studies [72][73][74][75][76].…”

Section: Geometry and Electronic Structure Of Co 1 /Mo 2 Cs 2 Monolayersupporting

confidence: 84%

“…MXenes have been found to have enormous applications within energy storage devices, catalysis, thermoelectric insulators, topological insulators [66,67]. Of particular interest is the finding that MXenes are promising materials for SAC substrate [68][69][70][71][72][73][74], especially because they are a type of stable, low-cost materials and can be easily prepared experimentally [75][76][77].…”

Section: Introductionmentioning

confidence: 99%

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Non-noble metal single-atom catalyst of Co1/MXene (Mo2CS2) for CO oxidation

Talib

Baskaran

et al. 2020

Sci. China Mater.

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MXene is a variety of new two-dimensional (2D) materials with early transition metal carbides, nitrides, and carbonitrides. Quantum chemical studies have been carried out on the geometries, electronic structures, stability and catalytic properties of a non-noble metal single-atom catalyst (SAC) with single Co atom anchored on MXene materials of Mo 2 CS 2. The Co adatom anchored on top of the Mo atom of this MXene is found to be rather stable, and this SAC is appropriate for CO oxidation. The charge transfers from the surface to the adsorbed CO and O 2 play a significant role in the activation of these molecules on Co 1 /Mo 2 CS 2. With this catalyst, the Eley-Rideal (ER), Langmuir-Hinshelwood (LH), and Termolecular Eley-Rideal (TER) mechanisms are explored for CO oxidation. We find that, while all the three mechanisms are feasible at low temperature, Co 1 /Mo 2 CS 2 possesses higher catalytic activity for CO oxidation through the TER mechanism that features an intriguing OC(OO)CO intermediate (IM) adsorbed on Co single atom. The calculated activation energy barriers of the rate-limiting step are 0.67 eV (TER), 0.78 eV (LH) and 0.88 eV (ER), respectively. The present study illustrates that it is promising to develop and design low-cost, non-noble metal SACs using MXene types of 2D materials.

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Section: Geometry and Electronic Structure Of Co 1 /Mo 2 Cs 2 Monolayersupporting

confidence: 84%

Section: Introductionmentioning

confidence: 99%

Non-noble metal single-atom catalyst of Co1/MXene (Mo2CS2) for CO oxidation

Talib

Baskaran

et al. 2020

Sci. China Mater.

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“…Thed iffusion barriers of the single atom Pf rom the initial hcp site to the next anchoring site are larger than 0.36 eV,which confirms that Psingle atoms are stabilized and immobilized on the supports. [26] In addition, the relative energy barrier required for the aggregation of two adjacent P atoms is calculated to be about 3.393 eV in Figure S17. This high energy barrier further demonstrates their stability and dispersion of Psingle atoms on Mo 2 C(001) facet, which can be supported by the experimental observations.…”

Section: Methodsmentioning

confidence: 99%

Non‐Metal Single‐Phosphorus‐Atom Catalysis of Hydrogen Evolution

Wang

Tian

et al. 2020

Angew Chem Int Ed

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Non‐metal‐based single‐atom catalysts (SACs) offer low cost, simple synthesis methods, and effective regulation for substrates. Herein, we developed a simplified pressurized gas‐assisted process, and report the first non‐metal single‐atom phosphorus with atomic‐level dispersion on unique single‐crystal Mo2C hexagonal nanosheet arrays with a (001) plane supported by carbon sheet (SAP‐Mo2C‐CS). The SAP‐Mo2C‐CS is structurally stable and shows exceptional electrocatalytic activity for the hydrogen evolution reaction (HER). A so‐called high‐active “window” based on the active sites of P atoms and their adjacent Mo atoms gives a ΔGH* close to zero for hydrogen evolution, which is the most ideal ΔGH* reported so far. Meanwhile, the moderate d‐band center value of SAP‐Mo2C‐CS can be also used as an ideal standard value to evaluate the HER performance in non‐metal‐based SACs.

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“…Thus, we examined the energy barriers of P diffusing on the support by the climbing‐image nudged‐elastic‐band method (CI‐NEB) in Figure 4 c (in the following part, the most stable hcp configuration as the main research object). The diffusion barriers of the single atom P from the initial hcp site to the next anchoring site are larger than 0.36 eV, which confirms that P single atoms are stabilized and immobilized on the supports [26] . In addition, the relative energy barrier required for the aggregation of two adjacent P atoms is calculated to be about 3.393 eV in Figure S17.…”

Section: Resultsmentioning

confidence: 77%