Journal ArticleDOI

# A metal-free polymeric photocatalyst for hydrogen production from water under visible light

01 Jan 2009-Nature Materials (Nature Publishing Group)-Vol. 8, Iss: 1, pp 76-80

TL;DR: It is shown that an abundant material, polymeric carbon nitride, can produce hydrogen from water under visible-light irradiation in the presence of a sacrificial donor.
Abstract: The production of hydrogen from water using a catalyst and solar energy is an ideal future energy source, independent of fossil reserves. For an economical use of water and solar energy, catalysts that are sufficiently efficient, stable, inexpensive and capable of harvesting light are required. Here, we show that an abundant material, polymeric carbon nitride, can produce hydrogen from water under visible-light irradiation in the presence of a sacrificial donor. Contrary to other conducting polymer semiconductors, carbon nitride is chemically and thermally stable and does not rely on complicated device manufacturing. The results represent an important first step towards photosynthesis in general where artificial conjugated polymer semiconductors can be used as energy transducers.
Topics: Energy source (59%), Hydrogen production (56%), Carbon nitride (55%), Solar energy (54%)
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Journal ArticleDOI
10 Nov 2010-Chemical Reviews
TL;DR: Approaches to Modifying the Electronic Band Structure for Visible-Light Harvesting and its Applications d0 Metal Oxide Photocatalysts 6518 4.4.1.
Abstract: 2.3. Evaluation of Photocatalytic Water Splitting 6507 2.3.1. Photocatalytic Activity 6507 2.3.2. Photocatalytic Stability 6507 3. UV-Active Photocatalysts for Water Splitting 6507 3.1. d0 Metal Oxide Photocatalyts 6507 3.1.1. Ti-, Zr-Based Oxides 6507 3.1.2. Nb-, Ta-Based Oxides 6514 3.1.3. W-, Mo-Based Oxides 6517 3.1.4. Other d0 Metal Oxides 6518 3.2. d10 Metal Oxide Photocatalyts 6518 3.3. f0 Metal Oxide Photocatalysts 6518 3.4. Nonoxide Photocatalysts 6518 4. Approaches to Modifying the Electronic Band Structure for Visible-Light Harvesting 6519

5,825 citations

Journal ArticleDOI
Wee-Jun Ong1, Lling-Lling Tan1, Yun Hau Ng2, Siek Ting Yong1  +1 moreInstitutions (2)
20 May 2016-Chemical Reviews
TL;DR: It is anticipated that this review can stimulate a new research doorway to facilitate the next generation of g-C3N4-based photocatalysts with ameliorated performances by harnessing the outstanding structural, electronic, and optical properties for the development of a sustainable future without environmental detriment.
Abstract: As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...

3,562 citations

Journal ArticleDOI
Juan Liu1, Yang Liu1, Naiyun Liu1, Yuzhi Han1  +7 moreInstitutions (2)
27 Feb 2015-Science
TL;DR: The design and fabrication of a metal-free carbon nanodot–carbon nitride (C3N4) nanocomposite is reported and its impressive performance for photocatalytic solar water splitting is demonstrated.
Abstract: The use of solar energy to produce molecular hydrogen and oxygen (H2 and O2) from overall water splitting is a promising means of renewable energy storage. In the past 40 years, various inorganic and organic systems have been developed as photocatalysts for water splitting driven by visible light. These photocatalysts, however, still suffer from low quantum efficiency and/or poor stability. We report the design and fabrication of a metal-free carbon nanodot-carbon nitride (C3N4) nanocomposite and demonstrate its impressive performance for photocatalytic solar water splitting. We measured quantum efficiencies of 16% for wavelength λ = 420 ± 20 nanometers, 6.29% for λ = 580 ± 15 nanometers, and 4.42% for λ = 600 ± 10 nanometers, and determined an overall solar energy conversion efficiency of 2.0%. The catalyst comprises low-cost, Earth-abundant, environmentally friendly materials and shows excellent stability.

2,877 citations

Journal ArticleDOI
Hua Tong1, Shuxin Ouyang1, Yingpu Bi1, Naoto Umezawa2  +3 moreInstitutions (2)
TL;DR: This article reviews state-of-the-art research activities in the field, focusing on the scientific and technological possibilities offered by photocatalytic materials, and highlights crucial issues that should be addressed in future research activities.
Abstract: Semiconductor photocatalysis has received much attention as a potential solution to the worldwide energy shortage and for counteracting environmental degradation. This article reviews state-of-the-art research activities in the field, focusing on the scientific and technological possibilities offered by photocatalytic materials. We begin with a survey of efforts to explore suitable materials and to optimize their energy band configurations for specific applications. We then examine the design and fabrication of advanced photocatalytic materials in the framework of nanotechnology. Many of the most recent advances in photocatalysis have been realized by selective control of the morphology of nanomaterials or by utilizing the collective properties of nano-assembly systems. Finally, we discuss the current theoretical understanding of key aspects of photocatalytic materials. This review also highlights crucial issues that should be addressed in future research activities.

2,873 citations

Journal ArticleDOI
Yong Wang1, Xinchen Wang1, Markus Antonietti1Institutions (1)
02 Jan 2012-Angewandte Chemie
TL;DR: The "polymer chemistry" of g-C(3)N(4) is described, how band positions and bandgap can be varied by doping and copolymerization, and how the organic solid can be textured to make it an effective heterogenous catalyst.
Abstract: Polymeric graphitic carbon nitride materials (for simplicity: g-C(3)N(4)) have attracted much attention in recent years because of their similarity to graphene. They are composed of C, N, and some minor H content only. In contrast to graphenes, g-C(3)N(4) is a medium-bandgap semiconductor and in that role an effective photocatalyst and chemical catalyst for a broad variety of reactions. In this Review, we describe the "polymer chemistry" of this structure, how band positions and bandgap can be varied by doping and copolymerization, and how the organic solid can be textured to make it an effective heterogenous catalyst. g-C(3)N(4) and its modifications have a high thermal and chemical stability and can catalyze a number of "dream reactions", such as photochemical splitting of water, mild and selective oxidation reactions, and--as a coactive catalytic support--superactive hydrogenation reactions. As carbon nitride is metal-free as such, it also tolerates functional groups and is therefore suited for multipurpose applications in biomass conversion and sustainable chemistry.

2,360 citations

##### References
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Journal ArticleDOI
Abstract: CASTEP Computer program / Density functional theory / Pseudopotentials / ab initio study / Plane-wave method / Computational crystallography Abstract. The CASTEP code for first principles electro- nic structure calculations will be described. A brief, non- technical overview will be given and some of the features and capabilities highlighted. Some features which are un- ique to CASTEP will be described and near-future devel- opment plans outlined.

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Kazuhiko Maeda1, Kentaro Teramura1, Daling Lu, Tsuyoshi Takata1  +3 moreInstitutions (2)
16 Mar 2006-Nature
TL;DR: An advance in the catalysis of the overall splitting of water under visible light is described: the new catalyst is a solid solution of gallium and zinc nitrogen oxide, modified with nanoparticles of a mixed oxide of rhodium and chromium, which functions as a promising and efficient photocatalyst in promoting the evolution of hydrogen gas.
Abstract: Enhancing catalytic performance holds promise for hydrogen production by water splitting in sunlight.

2,335 citations

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O. Khaselev1, John A. Turner1Institutions (1)
17 Apr 1998-Science
TL;DR: Direct water electrolysis was achieved with a novel, integrated, monolithic photoelectrochemical-photovoltaic design that splits water directly upon illumination; light is the only energy input.
Abstract: Direct water electrolysis was achieved with a novel, integrated, monolithic photoelectrochemical-photovoltaic design. This photoelectrochemical cell, which is voltage biased with an integrated photovoltaic device, splits water directly upon illumination; light is the only energy input. The hydrogen production efficiency of this system, based on the short-circuit current and the lower heating value of hydrogen, is 12.4 percent.

1,928 citations

Journal ArticleDOI
Karsten Reuter1, Matthias Scheffler1Institutions (1)
19 Dec 2001-Physical Review B
Abstract: Using density-functional theory we calculate the Gibbs free energy to determine the lowest-energy structure of a ${\mathrm{RuO}}_{2}(110)$ surface in thermodynamic equilibrium with an oxygen-rich environment. The traditionally assumed stoichiometric termination is only found to be favorable at low oxygen chemical potentials, i.e., low pressures and/or high temperatures. At a realistic O pressure, the surface is predicted to contain additional terminal O atoms. Although this O excess defines a so-called polar surface, we show that the prevalent ionic model, that dismisses such terminations on electrostatic grounds, is of little validity for ${\mathrm{RuO}}_{2}(110).$ Together with analogous results obtained previously at the (0001) surface of corundum-structured oxides, these findings on (110) rutile indicate that the stability of nonstoichiometric terminations is a more general phenomenon of transition metal oxide surfaces.

1,440 citations

Journal ArticleDOI
Kazuhiko Maeda and1, Kazunari Domen1Institutions (1)
Abstract: Overall water splitting to form hydrogen and oxygen over a heterogeneous photocatalyst using solar energy is a promising process for clean and recyclable hydrogen production in large-scale. In recent years, numerous attempts have been made for the development of photocatalysts that work under visible-light irradiation to efficiently utilize solar energy. This article presents recent research progress in the development of visible-light-driven photocatalysts, focusing on the refinement of non-oxide-type photocatalysts such as (oxy)nitrides and oxysulfides.

1,219 citations

### "A metal-free polymeric photocatalys..." refers background in this paper

• ...There are some cases where N 2 evolution and sulphur deposition are observed as a result of oxidative decomposition of the photocatalys...

[...]

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YearCitations
202268
20211,246
20201,165
20191,093
20181,036
2017903