Single‐Atom Pt as Co‐Catalyst for Enhanced Photocatalytic H<sub>2</sub> Evolution

Li, Yong; Bi, Wentuan; Zhang, Lei; Tao, Shi; Chu, Wei; Zhang, Qun; Luo, Yi; Wu, Changzheng; Xie, Yi

doi:10.1002/adma.201505281

Cited by 1,265 publications

(847 citation statements)

References 34 publications

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“…In the case of carbon nitride, the selective breaking of abundant hydrogen bonds in the intralayer framework not only extends visible light absorption range but also suppresses the radiative electron-hole recombination as demonstrated by Figure 4 , whose origin is the increased low-energy photon excitations and band-to-tail charge transfer processes induced by the increased band tails/localized states close to the band edges. In contrast, for the carbon nitride with broken hydrogen bonds the deposited Au particles with a relatively uniform particle size of around 10 nm (a small particle size of noble metal as co-catalyst favors the transfer of photoexcited electrons from a semiconductor to co-catalyst [ 35 ] ) are well dispersed through the whole carbon nitride particles. In addition to these electronic structure-induced favorable features, the abundant interconnected pores through the whole particles simultaneously formed by breaking hydrogen bonds play an important role in geometrically shortening the diffusion lengths of both the photoexcited electrons from the interior to edges of the layers and reactants from the surface to the interior of a particle along the interlayer galleries.…”

Section: Communicationmentioning

confidence: 64%

Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

et al. 2016

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Selective breaking of the hydrogen bonds of graphitic carbon nitride can introduce favorable features, including increased band tails close to the band edges and the creation of abundant pores. These features can simultaneously improve the three basic processes of photocatalysis. As a consequence, the photocatalytic hydrogen-generation activity of carbon nitride under visible light is drastically increased by tens of times.

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Section: Communicationmentioning

confidence: 64%

Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

et al. 2016

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“…Li et al [202] reported singleatom Pt as cocatalyst for enhanced photocatalytic H 2 evolution of gC 3 (Figure 17a) demonstrated that the Pt atoms are uniformly dispersed on the surface of gC 3 N 4 , and the sizes of 99.4% of Pt species are below 0.2 nm. As is well known, the heterogeneous catalytic reactions are surface reactions.…”

Section: G-c 3 N 4 /Metal Heterostructurementioning

confidence: 99%

g‐C₃N₄‐Based Heterostructured Photocatalysts

Wang

Jiang

et al. 2017

Advanced Energy Materials

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Thereafter, the photocatalytic degrada tion of polychlorobiphenyls [2] and photo electrocatalytic reduction of CO 2 into hydrocarbon compounds [3] in aqueous semiconductor suspensions greatly broad ened the applications of photocatalysis. Although the photocatalytic technology has got worldwide attention for its eco nomic, clean, safe, and renewable charac teristics, the photocatalytic performance of currently known photocatalysts is still far from commercial applications, especially in solartofuel conversion. [4][5][6][7][8][9][10][11] Generally, the photocatalytic reactions can be divided into three basic processes. First, the semiconductor photocatalysts absorb effective photons whose energy (h v ) is equal to or above their bandgap (E g ), resulting in the generation of electronhole pairs. Second, the photogenerated charge carriers separate and transfer to the surface of photocatalysts. Third, the photogenerated electrons and holes partic ipate in reactions of substances adsorbed on the surface of the photocatalysts. [12,13] Thus, the improvements of the three aforementioned processes play impor tant roles in enhancing the photocatalytic performance. Light absorption is the first essential step of photocatalysis process. The traditional anatase phase TiO 2 photocatalyst is active only under UV light with wavelength below 387 nm due to its wide bandgap (3.2 eV). However, solar energy is mainly concentrated in the visible light region, and UV light accounts for less than 4% of the solar spectrum. [7] In order to achieve maximum utilization efficiency of solar energy, the exploration of visiblelightresponsive photo catalysts is an urgent task. Graphitic carbon nitride (gC 3 N 4 ) as a promising visiblelightresponsive photocatalyst has received worldwide attention due to its fascinating merits, such as moderate bandgap (≈2.7 eV), proper electronic band structure, nontoxicity, low cost, good stability, and easy preparation. [14][15][16][17][18] Since the first report on photocatalytic H 2 evolution over gC 3 N 4 by Wang et al. in 2009, [19] research endeavors toward improving the photocatalytic performance of gC 3 N 4 based photocatalysts have formed a forefront of photocatalysis research. [20][21][22][23][24][25] Bulk gC 3 N 4 powder can be prepared by the thermal poly condensation of lowcost nitrogencontaining organic pre cursors, e.g., urea, thiourea, melamine, cyanamide, dicyan diamide, guanidine hydrochloride, and so on. [26][27][28][29][30][31][32] The pure bulk gC 3 N 4 prepared by this method suffers from several shortcomings, including low specific surface area, insufficient visible light utilization, and, particularly, rapid recombination Photocatalysis is considered as one of the promising routes to solve the energy and environmental crises by utilizing solar energy. Graphitic carbon nitride (g-C 3 N 4 ) has attracted worldwide attention due to its visible-light activity, facile synthesis from low-cost materials, chemical stability, and unique layered structure. However, the pure g-C 3 N 4 photocatalys...

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“…[6,7] Atomically dispersed catalysts comprising mononuclear metal complexes or single metal atoms provide as uitable model for atomic-level insight into reaction kinetics of the active site. [12] Recently,t he synthetic cobalt-based complexes containing square planar-like "Co 1 -N 4 "single active site have been explored as effective H 2 -evolution catalysts. [12] Recently,t he synthetic cobalt-based complexes containing square planar-like "Co 1 -N 4 "single active site have been explored as effective H 2 -evolution catalysts.…”

mentioning

confidence: 99%

“…[20] Theunsaturated Nwith an electron lone pair is an ideal anchoring site for immobilizing metal ions into C 3 N 4 framework. [12] Co ALD was performed using bis(cyclo-pentadienyl)cobalt, Co(Cp) 2 ,followed by O 3 treatment under as hort time of 150 sa nd ar elatively low temperature of 150 8 8Ct or emove the surface Cp ligand. It should be noted that the phosphidation and Co ALD process would not largely influence the morphology and main matrix network of g-C 3 N 4 (Supporting Information, Figures S1, S2).…”

mentioning

confidence: 99%

Atomic‐Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co₁‐N₄ Single‐Site Photocatalyst

et al. 2017

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Knowledge of the photocatalytic H evolution mechanism is of great importance for designing active catalysts toward a sustainable energy supply. An atomic-level insight, design, and fabrication of single-site Co -N composite as a prototypical photocatalyst for efficient H production is reported. Correlated atomic characterizations verify that atomically dispersed Co atoms are successfully grafted by covalently forming a Co -N structure on g-C N nanosheets by atomic layer deposition. Different from the conventional homolytic or heterolytic pathway, theoretical investigations reveal that the coordinated donor nitrogen increases the electron density and lowers the formation barrier of key Co hydride intermediate, thereby accelerating H-H coupling to facilitate H generation. As a result, the composite photocatalyst exhibits a robust H production activity up to 10.8 μmol h , 11 times higher than that of pristine counterpart.

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Single‐Atom Pt as Co‐Catalyst for Enhanced Photocatalytic H₂ Evolution

Cited by 1,265 publications

References 34 publications

Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

g‐C₃N₄‐Based Heterostructured Photocatalysts

Atomic‐Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co₁‐N₄ Single‐Site Photocatalyst

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Single‐Atom Pt as Co‐Catalyst for Enhanced Photocatalytic H2 Evolution

Cited by 1,265 publications

References 34 publications

Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

g‐C3N4‐Based Heterostructured Photocatalysts

Atomic‐Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co1‐N4 Single‐Site Photocatalyst

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Single‐Atom Pt as Co‐Catalyst for Enhanced Photocatalytic H₂ Evolution

g‐C₃N₄‐Based Heterostructured Photocatalysts

Atomic‐Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co₁‐N₄ Single‐Site Photocatalyst