Thiomolybdate [Mo3S13]2−nanocluster: a molecular mimic of MoS2active sites for highly efficient photocatalytic hydrogen evolution

Lei, Yonggang; Yang, Meiqun; Hou, Jianhua; Wang, Fang; Cui, Entian; Kong, Chao; Min, Shixiong

doi:10.1039/c7cc08178b

Cited by 60 publications

(44 citation statements)

References 30 publications

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“…Such low activities are consistent with previous reports for perovskite‐based photocatalysis without help of stabilizer and cocatalyst . [Mo 3 S 13 ] 2 2− nanoclusters as the cocatalyst have an excellent hydrogen evolution activity and stability in acid condition . The XRD of Mo 3 S 13 2− treated by HBr solution was shown in Figure S7.…”

Section: Resultssupporting

confidence: 91%

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Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H₂ generation

Yue

Zhang

Yang

et al. 2020

EcoMat

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Various optoelectronic applications of organic inorganic hybrid lead halide perovskites are challenged by their stability. The photocatalytic stability of lead halide perovskites are so low that chemical stabilizer such as H3PO2 are required in their applications. We report a postsynthesis potassium stabilization on methylammonium lead bromide (MAPbBr3) to form K‐MAPbBr3 by doping K cation and depositing KBr layers. In absence of any stabilizer, this stable K‐MAPbBr3 perovskite can exhibit an unprecedented high photostability even after 200 hours continuous photocatalytic H2 generation. Impressively, the K‐MAPbBr3 cocatalyzed with Mo3S132− nanoclusters achieves a high apparent quantum efficiency up to 18.3% at 450 nm for photocatalytic H2 generation. The mechanism study reveals that the photogeneration of Pb0 and Br0 defects are effectively inhibited in K‐MAPbBr3, which makes it a robust photocatalyst for H2 generation. These findings will inspire the development of stable organic‐inorganic hybrid perovskites for photocatalysis and other optoelectronic applications.

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Section: Resultssupporting

confidence: 91%

“…[7][8][9] [Mo 3 S 13 ] 2 2− nanoclusters as the cocatalyst have an excellent hydrogen evolution activity and stability in acid condition. [24][25][26] The XRD of Mo 3 S 13 2− treated by HBr solution was shown in Figure S7. The crystal structure can be assigned as a standard (NH 4 ) 2 Mo 3 S 13 ÁnH 2 O XRD data (JCPDS No.…”

Section: Resultsmentioning

confidence: 99%

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H₂ generation

Yue

Zhang

Yang

et al. 2020

EcoMat

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“…12 Recently, homogeneous photocatalytic HER activity of thiomolybdate [Mo 3 S 13 ] 2– was reported. 13 In a subsequent study, it was shown that under catalytic conditions, terminal disulfide ligands exchange with solvent (H 2 O) over time and influence the catalytic activity. 14 In particular, partial exchange of terminal disulfides (S 2 2– ) with aqua ligands leads to [Mo 3 S (13- x ) (H 2 O) x ] ( x -2)+ ( x = 2, 4) which could be identified as the most active catalytic species in solution.…”

Section: Introductionmentioning

confidence: 99%

Structural Properties of Gas Phase Molybdenum Sulfide Clusters [Mo₃S₁₃]^2–, [HMo₃S₁₃]⁻, and [H₃Mo₃S₁₃]⁺ as Model Systems of a Promising Hydrogen Evolution Catalyst

et al. 2018

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Amorphous molybdenum sulfide (MoS x ) is a potent catalyst for the hydrogen evolution reaction (HER). Since mechanistic investigations on amorphous solids are particularly difficult, we use a bottom-up approach and study the [Mo 3 S 13 ] 2– nanocluster and its protonated forms. The mass selected pure [Mo 3 S 13 ] 2– as well as singly and triply protonated [HMo 3 S 13 ] − and [H 3 Mo 3 S 13 ] + ions, respectively, were investigated by a combination of collision induced dissociation (CID) experiments and quantum chemical calculations. A rich variety of H x S y elimination channels was observed, giving insight into the structural flexibility of the clusters. In particular, it was calculated that the observed clusters tend to keep the Mo 3 ring structure found in the bulk and that protons adsorb primarily on terminal disulfide units of the cluster. Mo–H bonds are formed only for quasi-linear species with Mo centers featuring empty coordination sites. Protonation leads to increased cluster stability against CID. The rich variety of CID dissociation products for the triply protonated [H 3 Mo 3 S 13 ] + ion, however, suggests that it has a large degree of structural flexibility, with roaming H/SH moieties, which could be a key feature of MoS x to facilitate HER catalysis via a Volmer−Heyrovsky mechanism.

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“…XPS was used to analyze the chemical bonds on the surface of those samples, as shown in Supplementary Figure S1 and (Quinlan et al, 2016;Li et al, 2018b;Ni et al, 2018;Song et al, 2019;Yue et al, 2019;Han et al, 2020), respectively. The Mo 3 d and S 2s highly deconvoluted spectra of F-MoS 2 @NC-0.8 (Figure 3B) showed the three fitted peaks at 235.7, 232.5 and 229.4 eV are related to Mo 6+ −O, Mo 3d 3/2 and Mo 3d 5/2 (Feng et al, 2015;Ahn et al, 2018;Lei et al, 2018). It should be noted that the slight surface oxidation of MoS 2 could cause the existence of Mo 6+ −O.…”

Section: Resultsmentioning

confidence: 97%

N-Doped Carbon Boosted the Formation of Few-Layered MoS2 for High-Performance Lithium and Sodium Storage

Zhou

Lü

et al. 2021

Front. Mater.

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Molybdenum sulfide (MoS2) has become a potential anode of lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) due to its high theoretical capacity and low cost. However, the volume expansion, poor electrical conductivity and dissolution of polysulfides in the electrolyte during the cycling process severely limited its applications. Herein, few-layered MoS2@N-doped carbon (F-MoS2@NC) was synthesized through a facile solvothermal and annealing process. It was found that the addition of N-doped carbon precursor could significantly promote the formation of few-layered MoS2 and improve the performances of lithium and sodium storage. A high reversible capacity of 482.6 mA h g−1 at a high current density of 2000 mA g−1 could be obtained for LIBs. When used as anode material for SIBs, F-MoS2@NC hybrids could maintain a reversible capacity of 171 mA h g−1 at a high current density of 1,000 mA g−1 after 600 cycles. This work should provide new insights into carbon hybrid anode materials for both LIBs and SIBs.

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Thiomolybdate [Mo₃S₁₃]²⁻nanocluster: a molecular mimic of MoS₂active sites for highly efficient photocatalytic hydrogen evolution

Cited by 60 publications

References 30 publications

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H₂ generation

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H₂ generation

Structural Properties of Gas Phase Molybdenum Sulfide Clusters [Mo₃S₁₃]^2–, [HMo₃S₁₃]⁻, and [H₃Mo₃S₁₃]⁺ as Model Systems of a Promising Hydrogen Evolution Catalyst

N-Doped Carbon Boosted the Formation of Few-Layered MoS2 for High-Performance Lithium and Sodium Storage

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Thiomolybdate [Mo3S13]2−nanocluster: a molecular mimic of MoS2active sites for highly efficient photocatalytic hydrogen evolution

Cited by 60 publications

References 30 publications

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H2 generation

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H2 generation

Structural Properties of Gas Phase Molybdenum Sulfide Clusters [Mo3S13]2–, [HMo3S13]−, and [H3Mo3S13]+ as Model Systems of a Promising Hydrogen Evolution Catalyst

N-Doped Carbon Boosted the Formation of Few-Layered MoS2 for High-Performance Lithium and Sodium Storage

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Thiomolybdate [Mo₃S₁₃]²⁻nanocluster: a molecular mimic of MoS₂active sites for highly efficient photocatalytic hydrogen evolution

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H₂ generation

Potassium stabilization of methylammonium lead bromide perovskite for robust photocatalytic H₂ generation

Structural Properties of Gas Phase Molybdenum Sulfide Clusters [Mo₃S₁₃]^2–, [HMo₃S₁₃]⁻, and [H₃Mo₃S₁₃]⁺ as Model Systems of a Promising Hydrogen Evolution Catalyst