Surface step decoration of isolated atom as electron pumping: Atomic-level insights into visible-light hydrogen evolution

Wu, Xin; Zhang, Huabin; Dong, Juncai; M, Qiu; Kong, Jintao; Zhang, Yongfan; Yang, Li; Xu, Guilan; Zhang, Jian; Ye, Jinhua

doi:10.1016/j.nanoen.2017.12.039

Cited by 134 publications

(126 citation statements)

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“…[1][2][3] As an attractive strategy to utilize solar energy, photocatalytic water splitting can generate clean hydrogen fuel, which can be utilized for many applications such as industrial hydrogenation reactions and fuel cells. [8][9][10][11] However, most semiconductor materials exhibit relatively low activity even with the assistance of sacrificial agents. [8][9][10][11] However, most semiconductor materials exhibit relatively low activity even with the assistance of sacrificial agents.…”

Section: Photocatalysismentioning

confidence: 99%

“…[21] Moreover, when loaded onto semiconductor photocatalysts, metal oxide clusters can induce discrete energy bands to trap charge carriers and promote the separation of electrons and holes. [8][9][10][11] However, most semiconductor materials exhibit relatively low activity even with the assistance of sacrificial agents. [22][23][24] Therefore, it is essential to establish a synthetic method to precisely control the configuration of clusters decorated on the surface of semiconductor photocatalysts at atomic level.…”

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confidence: 99%

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Ultrasmall MoO_x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

et al. 2018

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of semiconductor photocatalysts to retard the recombination of charge carriers and enhance surface reaction rates. [13][14][15] Among various kinds of cocatalysts, Pt often shows the best performance. However, practical application of Pt-based cocatalysts is limited by their scarcity and high cost. [16] Therefore, development of highly active and cost-efficient alternatives to Pt is urgently needed. A large number of transition metals (e.g., iron, cobalt, nickel, molybdenum, and tungsten) and their derivative compounds have been studied. Fu and colleagues have integrated CdS with MoS 2 and obtained much improved hydrogen evolution activity. [17] However, the performances of which are still far from satisfactory because of the low active surface areas and sluggish separation of electron-hole pairs. [18][19][20] Thus, designing novel materials which can address these problems may lead to the discovery of non-noble metal cocatalysts with enhanced performance. Metal oxide clusters, constructed by a small number of atoms, can largely expose active metal sites. [21] Moreover, when loaded onto semiconductor photocatalysts, metal oxide clusters can induce discrete energy bands to trap charge carriers and promote the separation of electrons and holes. Regarding such unique properties, cluster cocatalysts show the potential to boost the activity of semiconductor photocatalysts for solar water splitting.The performance of cluster cocatalysts is significantly influenced by the number and coordination environment of the active atoms. [22][23][24] Therefore, it is essential to establish a synthetic method to precisely control the configuration of clusters decorated on the surface of semiconductor photocatalysts at atomic level. [25,26] Herein, a bottom-up strategy is developed to decorate ultrasmall molybdenum-oxygen (MoO x ) clusters onto the surface of CdS nanowires (NWs). The decorated clusters with finely controlled size and configuration greatly enhance the photocatalytic H 2 evolution efficiency of CdS NWs.CdS NWs are first synthesized through a solvothermal approach. [27] X-ray diffraction (XRD) pattern of as-prepared sample shows characteristic peaks of CdS with hexagonal wurtzite crystal structure ( Figure S1, Supporting Information). Field-emission scanning electron microscope (FESEM), transmission electron microscope (TEM), and high-resolution TEM (HRTEM) images indicate the successful synthesis of CdS NWs with good crystallinity (Figure S2, Supporting Information). The average diameter of the CdS NWs is about 75 nm (Figure S3, Supporting Information). MoO x clusters are then decorated To enhance the performance of semiconductor photocatalysts, cocatalysts are used to accelerate surface reactions. Herein, ultrasmall molybdenumoxygen (MoO x ) clusters are developed as a novel non-noble cocatalyst, which significantly promotes the photocatalytic hydrogen generation rate of CdS nanowires (NWs). As indicated by extended X-ray absorption fine structure analysis, direct bonds are formed between CdS NWs and MoO x clusters,...

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Section: Photocatalysismentioning

confidence: 99%

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Ultrasmall MoO_x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

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“…42 For example, abundant Pt-S bonds are formed between unsaturated sulfur atoms from CdS and isolated platinum atoms. 43 It was also found that Pd atom strongly interacts with TiO2 to maintain its stability as well. 44 Such interaction plays a crucial role in preventing the sintering of the cotatalyst and, in return, improves the stability of the cocatalyst.…”

Section: Introductionmentioning

confidence: 99%

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Doronkin

et al. 2019

Journal of Catalysis

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As an important byproduct during natural gas exploitation, green utilization of hydrogen sulfide (H2S) by photocatalysis has offered us the possibility for production of clean hydrogen (H2) from H2S with low energy consumption. In this work, we have successfully introduced well-dispersed palladium sulfide (PdS) which is preferably loaded on In2S3 of MnS/In2S3 composite for improved photocatalytic hydrogen evolution from H2S aqueous solution. In contrast to binary MnS/In2S3, ternary MnS/In2S3/PdS has exhibited a remarkable and stable hydrogen production rate of 22.7 mmol g-1 h-1 with an apparent quantum yield of 34 % at around 395 nm. A comprehensive structure characterization of the ternary composite including scanning transmission electron microscopy (STEM) and X-ray absorption spectroscopy (XAS) in combination with theoretical calculations confirm the good dispersion of PdS in the composite. Moreover, we discovered that PdS preferably interact with In2S3 rather than MnS in the composite through Pd-SIn bond on the interface of the two. Photoluminescence (PL) spectra, surface photovoltage (SPV) spectra together with transient photocurrent and electrochemical impedance spectra (EIS) demonstrate the advantage of PdS for promoting the charge separation. Due to the corrosion-resistant nature of PdS in H2S-rich reaction media, MnS/In2S3/PdS present good stability as well. This work sheds light on the positive effect on the enhanced activity and stability of the corresponding system resulting from the preferable anchoring of highly dispersed PdS on In2S3 in the composite by chemical Pd-SIn bond. Not only the high dispersion but also the preferable anchoring of the cocatalyst in the composite could hence inspire people for more rational designs of ternary composite in future.

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“…[6] As a clean energy carrier, H2 has the highest energy density (120-142 MJ/kg) in comparison to any other fuels without carbon trace. [7][8][9][10] Therefore, the production of H2 from H2S is beneficial for both the abatement of the toxic pollutant and producing clean energy.…”

Section: Introductionmentioning

confidence: 99%

Novel MnS/(InxCu1-x)2S3 composite for robust solar hydrogen sulphide splitting via the synergy of solid solution and heterojunction

Dan

Wei

Doronkin

et al. 2019

Applied Catalysis B: Environmental

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Surface step decoration of isolated atom as electron pumping: Atomic-level insights into visible-light hydrogen evolution

Cited by 134 publications

References 65 publications

Ultrasmall MoO_x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

Ultrasmall MoO_x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Novel MnS/(InxCu1-x)2S3 composite for robust solar hydrogen sulphide splitting via the synergy of solid solution and heterojunction

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Surface step decoration of isolated atom as electron pumping: Atomic-level insights into visible-light hydrogen evolution

Cited by 134 publications

References 65 publications

Ultrasmall MoOx Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

Ultrasmall MoOx Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Novel MnS/(InxCu1-x)2S3 composite for robust solar hydrogen sulphide splitting via the synergy of solid solution and heterojunction

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Ultrasmall MoO_x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution

Ultrasmall MoO_x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution