Mo thio and oxo-thio molecular complexes film as self-healing catalyst for photocatalytic hydrogen evolution on 2D materials

Barbosa, Juliana Barros; Taberna, Pierre Louis; Bourdon, Valérie; Gerber, Iann C.; Poteau, Romuald; Balocchi, Andréa; Marie, X.; Esvan, Jérôme; Puech, Pascal; Barnabé, Antoine; Vieira, Lucianna Da Gama Fernandes; Moraru, Ionut-Tudor; Chane‐Ching, Jean‐Yves

doi:10.1016/j.apcatb.2020.119288

Cited by 11 publications

(22 citation statements)

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“…Because charge carrier collection was shown to be a crucial point to achieve high photoelectrochemical performances in 3D nanoporous architectures constructed from 2D nanosheets, [35–37] a strategy based on patch‐like, layered hetero‐structures allowing the preservation of the high surface area was recently proposed. These patch‐like heterostructures include WSe 2 nanoflakes partially coated both with graphene nanosheets [38–40] to improve charge collection and with a healing co‐catalyst film [17,22] . Following these first results on p‐WSe 2, [17,22] we investigate herein a series of films composed of p‐WS 2 nanoflake building blocks.…”

Section: Introductionmentioning

confidence: 99%

“…These patch‐like heterostructures include WSe 2 nanoflakes partially coated both with graphene nanosheets [38–40] to improve charge collection and with a healing co‐catalyst film [17,22] . Following these first results on p‐WSe 2, [17,22] we investigate herein a series of films composed of p‐WS 2 nanoflake building blocks. In addition to being an environmentally friendly material, p‐WS 2 was selected to enrich the 2D TMDC materials library, thus offering a larger range of bandgap and HER onset potentials for the design of future tandem cells.…”

Section: Introductionmentioning

confidence: 99%

“…2D materials, including transition metal dichalcogenides (TMDC), [14] C 3 N 4 , [15] and Mxenes, [16] displaying unique light absorption properties and appropriate band energy levels for the photocatalytic production of hydrogen represent building blocks of great interest. Despite recent interesting results in defect chemistry control [17] as well as heterojunction formation and properties, [18,19] the large‐scale development of the 2D photoactive films will require numerous improvements and increased performances. Since TMDC in bulk form [20,21] have previously demonstrated high photocatalytic performances for the hydrogen evolution reaction (HER), their 2D nanoflakes counterparts [17,22–24] have attracted increased attention for the photocatalytic water splitting.…”

Section: Introductionmentioning

confidence: 99%

“…Despite recent interesting results in defect chemistry control [17] as well as heterojunction formation and properties, [18,19] the large‐scale development of the 2D photoactive films will require numerous improvements and increased performances. Since TMDC in bulk form [20,21] have previously demonstrated high photocatalytic performances for the hydrogen evolution reaction (HER), their 2D nanoflakes counterparts [17,22–24] have attracted increased attention for the photocatalytic water splitting. Nevertheless, high defect density and poor optoelectronic quality of these 2D materials have been reported [25,26] .…”

Section: Introductionmentioning

confidence: 99%

“…Nevertheless, the corresponding process routes involve 2D materials prepared at relatively low temperatures ( T <200 °C) [34] yielding films displaying poor optoelectronic quality not appropriate for photoactive materials. In contrast, nanosheets prepared from exfoliation of crystals synthesized at high temperature were shown to be suitable materials [17,23,24] . Using the bottom‐up strategy, close‐packed films prepared by self‐assembling in fluid/fluid (vs. fluid/air) interfaces were recently proposed [23] .…”

Section: Introductionmentioning

confidence: 99%

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Mitigation of Edge and Surface States Effects in Two‐Dimensional WS₂ for Photocatalytic H₂ Generation

et al. 2022

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Large scale development of the 2D transition metal dichalcogenides (TMDC) relies on landmark improvement in performance, which could emerge from nanostructuration. Using p-WS 2 nanoflakes with different degrees of exfoliation and fracturing, perspectives were provided to develop highsurface-area 2D p-WS 2 films for the photocatalytic hydrogen generation. The critical role of inter-nanoflakes contacts within high-surface-area 2D films was demonstrated, highlighting the benefit of plane/plane versus edge/plane contacts. Evidence of the high density of surface states displayed by these 2D films was provided through electrochemical measurements. In addition to operating as recombination centers, the surface states were shown to give rise to deleterious Fermi-level pinning (FLP), which dramatically decreased the efficiency of charge carrier separation. Lastly, promising strategies yielding FLP suppression via surface states modification were proposed. In particular, use of a multifunctional ultrathin film displaying healing, catalytic, and n-type semiconduction properties was shown to greatly enhance charge carrier separation and transport to the photo-electrode/electrolyte interface. When the 2D photoelectrodes were fabricated with the above prerequisites (i. e., a high proportion of plane/plane contacts and a successful surface states chemical modification), a photocurrent up to 4.5 mA cm À 2 was achieved for the first time on 2D p-WS 2 photocathodes for hydrogen generation.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Mitigation of Edge and Surface States Effects in Two‐Dimensional WS₂ for Photocatalytic H₂ Generation

et al. 2022

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Thiomolybdate Clusters: From Homogeneous Catalysis to Heterogenization and Active Sites

Batool,

Langer,

Myakala

et al. 2023

Advanced Materials

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Thiomolybdates are molecular molybdenum‐sulfide clusters formed from Mo centers and sulfur‐based ligands. For decades, they have attracted the interest of synthetic chemists due to their unique structures and their relevance in biological systems, e.g., as reactive sites in enzymes. More recently, thiomolybdates have been explored from the catalytic point of view and applied as homogeneous and molecular mimics of heterogeneous molybdenum sulfide catalysts. This review summarizes prominent examples of thiomolybdate‐based electro‐ and photocatalysis and provides a comprehensive analysis of their reactivities under homogeneous and heterogenized conditions. Active sites of thiomolybdates relevant for the hydrogen evolution reaction (HER) are examined, aiming to shed light on the link between cluster structure and performance. The shift from solution‐phase to surface‐supported thiomolybdates is discussed with a focus on applications in electrocatalysis and photocatalysis. The outlook highlights current trends and emerging areas of thiomolybdate research, ending with a summary of challenges and key takeaway messages based on the state‐of‐the‐art research.This article is protected by copyright. All rights reserved

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Semi‐Synthetic Chlorophyll‐Carotenoid Dyad for Dye‐Sensitized Photocatalytic Hydrogen Evolution

Liu

Chen

et al. 2021

Adv Materials Inter

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attractive and challenging researches in the field of artificial photosynthesis. [1][2][3] Photocatalytic hydrogen evolution (PHE) has been in the spotlight as it is a highly prospective approach to convert and store the solar energy into hydrogen energy efficiently to meet future global energy demand. Thus development of photocatalysis for PHE is considered to be a matter of central focus to solve the problem of energy shortage and environmental pollution. [4][5][6] PHE systems based on various kinds of semiconductors have been extensively investigated so far, [7,8] among which Pt/TiO 2 has been regarded as one of the most major photocatalysts. [9][10][11][12][13] To overcome the inherent defects of TiO 2 such as large band gap which leads to low photocatalytic efficiency, some research groups reported the development of dye-sensitized Pt/TiO 2 photocatalysts for hydrogen evolution. [14][15][16][17] A recent trend for sensitizing Pt/TiO 2 is the use of metal-free organic dyes with strong absorptivity and panchromatic sensitization properties. [18][19][20] For example, perylene-quinoxaline, [21] porphyrin-BODIPY, [22] phenothiazine-BODIPY, [23] thienopyrazine-triarylamine, [24] or multicarbazole [25] have been developed as covalently-linked multichromophore sensitizers for Pt/TiO 2 -based catalysts to realize efficient light absorption. In this context, we recently reported a dyad sensitizer of chlorophyll derivative connected with indoline dye for panchromatic PHE. [26] The high photocatalytic activity of dyad was attributed to not only an excellent A chlorin-carotenoid dyad Dyad-COOH possessing a C3 2 -carboxylic acid group and a carotenoid moiety at the terminal end of C17-substituent is synthesized from naturally occurring chlorophyll-a as a new sensitizer for photocatalytic hydrogen evolution (PHE). Under the same experimental conditions, a maximum turnover number (TON) of PHE based on Dyad-COOH/Pt/TiO 2 is much higher than those of Pt/TiO 2 -based photocatalysts sensitized by the corresponding chlorin carboxylic acid (Chl-COOH) without carotenoid side chain, sole carotenoic acid (Car-COOH), or their 1:1 (mol/mol) mixture. By coadsorbing different types of carboxylic acid, the TON of Chl-COOH is found to be increased probably due to the suppression of chlorin aggregates on the TiO 2 surface. The Dyad-COOH/Pt/TiO 2 exhibits excellent photocatalytic performance with the hydrogen evolution of 9147 µmol g −1 h −1 with TON of 425 when 43 µmol g −1 of dye is loaded on the Pt/TiO 2 catalyst, while a better TON of 556 is achieved by preparing the photocatalyst with 10 µmol g −1 of Dyad-COOH. This study provides new ideas for utilizing traditional photosynthetic dyes to a low-cost and highly-efficient photosensitizer for PHE.

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Mo thio and oxo-thio molecular complexes film as self-healing catalyst for photocatalytic hydrogen evolution on 2D materials

Cited by 11 publications

References 66 publications

Mitigation of Edge and Surface States Effects in Two‐Dimensional WS₂ for Photocatalytic H₂ Generation

Mitigation of Edge and Surface States Effects in Two‐Dimensional WS₂ for Photocatalytic H₂ Generation

Thiomolybdate Clusters: From Homogeneous Catalysis to Heterogenization and Active Sites

Semi‐Synthetic Chlorophyll‐Carotenoid Dyad for Dye‐Sensitized Photocatalytic Hydrogen Evolution

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Mo thio and oxo-thio molecular complexes film as self-healing catalyst for photocatalytic hydrogen evolution on 2D materials

Cited by 11 publications

References 66 publications

Mitigation of Edge and Surface States Effects in Two‐Dimensional WS2 for Photocatalytic H2 Generation

Mitigation of Edge and Surface States Effects in Two‐Dimensional WS2 for Photocatalytic H2 Generation

Thiomolybdate Clusters: From Homogeneous Catalysis to Heterogenization and Active Sites

Semi‐Synthetic Chlorophyll‐Carotenoid Dyad for Dye‐Sensitized Photocatalytic Hydrogen Evolution

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Mitigation of Edge and Surface States Effects in Two‐Dimensional WS₂ for Photocatalytic H₂ Generation

Mitigation of Edge and Surface States Effects in Two‐Dimensional WS₂ for Photocatalytic H₂ Generation