Functional carbon nitride materials for water oxidation: from heteroatom doping to interface engineering

Nanoscale ◽  
2020 ◽  
Vol 12 (13) ◽  
pp. 6937-6952 ◽  
Author(s):  
Huayang Zhang ◽  
Wenjie Tian ◽  
Xiaoguang Duan ◽  
Hongqi Sun ◽  
Yonglong Shen ◽  
...  
Keyword(s):  
Water Oxidation ◽  
Carbon Nitride ◽  
Interface Engineering ◽  
Intrinsic Structure ◽  
Heteroatom Doping ◽  
Structure Activity Relationships ◽  
Structure Activity ◽  
Polymeric Carbon ◽  
Chemical Water ◽  
Carbon Nitride Materials

Strategies for modifying polymeric carbon nitrides and their intrinsic structure–activity relationships for photo-, electro-, and photoelectro-chemical water oxidation are discussed.

scholarly journals Single-atom cobalt-hydroxyl modification of polymeric carbon nitride for highly enhanced photocatalytic water oxidation: ball milling increased single atom loading

2022 ◽  
Author(s):  
Fei Yu ◽  
Tingting Huo ◽  
Quanhua Deng ◽  
Guoan Wang ◽  
Yuguo Xia ◽  
...  
Keyword(s):  
Ball Milling ◽  
Water Splitting ◽  
Oxygen Evolution ◽  
Oxygen Evolution Reaction ◽  
Water Oxidation ◽  
Carbon Nitride ◽  
Single Atom ◽  
Overall Water Splitting ◽  
Polymeric Carbon

Expediting the oxygen evolution reaction (OER) is the key to achieving efficient photocatalytic overall water splitting. Herein, single-atom Co−OH modified polymeric carbon nitride (Co-PCN) was synthesized with single-atom loading increased...

scholarly journals Solar Energy Harvesting with Carbon Nitrides: Do We Understand the Mechanism?

2018 ◽  
Author(s):  
Wolfgang Domcke ◽  
Johannes Ehrmaier ◽  
Andrzej L. Sobolewski
Keyword(s):  
Excited State ◽  
Solar Energy ◽  
Water Molecule ◽  
Hydrogen Evolution ◽  
Water Splitting ◽  
Hydroxyl Radicals ◽  
Carbon Nitride ◽  
Carbon Nitrides ◽  
Polymeric Carbon ◽  
Carbon Nitride Materials

The photocatalytic splitting of water into molecular hydrogen and molecular oxygen with sunlight is the dream reaction for solar energy conversion. Since decades, transition-metal-oxide semiconductors and supramolecular organometallic structures have been extensively explored as photocatalysts for solar water splitting. More recently, polymeric carbon nitride materials consisting of triazine or heptazine building blocks have attracted considerable attention as hydrogen-evolution photocatalysts. The mechanism of hydrogen evolution with polymeric carbon nitrides is discussed throughout the current literature in terms of the familiar concepts developed for photoelectrochemical water splitting with semiconductors since the 1970s. We discuss in this perspective an alternative mechanistic paradigm for photoinduced water splitting with carbon nitrides, which focusses on the specific features of the photochemistry of aromatic N-heterocycles in aqueous environments. It is shown that a water molecule which is hydrogen-bonded to an N-heterocycle can be decomposed into hydrogen and hydroxyl radicals by two simple sequential photochemical reactions. This concept is illustrated by first-principles calculations of excited-state reaction paths and their energy profiles for hydrogen-bonded complexes of pyridine, triazine and heptazine with a water molecule. It is shown that the excited-state hydrogen-transfer and hydrogen-detachment reactions are essentially barrierless, in sharp contrast to water oxidation in the electronic ground state, where high barriers prevail. We also discuss in some detail the products of possible reactions of the highly reactive hydroxyl radicals with the chromophores. We hypothesize that the challenge of efficient solar hydrogen generation with carbon-nitride materials is less the decomposition of water as such, but rather the controlled recombination of the photogenerated radicals to the closed-shell products H2 and H2O2.

Molecular ruthenium water oxidation catalysts carrying non-innocent ligands: mechanistic insight through structure–activity relationships and quantum chemical calculations

2016 ◽  
Vol 6 (5) ◽  
pp. 1306-1319 ◽  
Author(s):  
Markus D. Kärkäs ◽  
Rong-Zhen Liao ◽  
Tanja M. Laine ◽  
Torbjörn Åkermark ◽  
Shams Ghanem ◽  
...  
Keyword(s):  
Quantum Chemical Calculations ◽  
Water Oxidation ◽  
Quantum Chemical ◽  
Oxidation Catalysis ◽  
Oxidation Catalysts ◽  
Structure Activity Relationships ◽  
Structure Activity ◽  
Mechanistic Insight ◽  
Insight Into

Herein is highlighted how structure–activity relationships can be used to provide mechanistic insight into H2O oxidation catalysis.

scholarly journals Using nickel manganese oxide catalysts for efficient water oxidation

2015 ◽  
Vol 51 (24) ◽  
pp. 5005-5008 ◽  
Author(s):  
Prashanth W. Menezes ◽  
Arindam Indra ◽  
Ophir Levy ◽  
Kamalakannan Kailasam ◽  
Vitaly Gutkin ◽  
...  
Keyword(s):  
Manganese Oxide ◽  
Water Oxidation ◽  
Oxide System ◽  
Oxide Catalysts ◽  
Structure Activity Relationships ◽  
Manganese Oxide Catalysts ◽  
Structure Activity ◽  
Nickel Manganese

Here we explore the nickel manganese oxide system for efficient water oxidation and their structure–activity relationships.

Gradient sulfur doping along polymeric carbon nitride films as visible light photoanodes for the enhanced water oxidation

2020 ◽  
Vol 268 ◽  
pp. 118398 ◽  
Author(s):  
Yuanxing Fang ◽  
Xiaochun Li ◽  
Yan Wang ◽  
Cristina Giordano ◽  
Xinchen Wang
Keyword(s):  
Visible Light ◽  
Water Oxidation ◽  
Carbon Nitride ◽  
Sulfur Doping ◽  
Polymeric Carbon

scholarly journals Solar Energy Harvesting with Carbon Nitrides: Do We Understand the Mechanism?

2018 ◽  
Author(s):  
Wolfgang Domcke ◽  
Johannes Ehrmaier ◽  
Andrzej L. Sobolewski
Keyword(s):  
Excited State ◽  
Solar Energy ◽  
Water Molecule ◽  
Hydrogen Evolution ◽  
Water Splitting ◽  
Hydroxyl Radicals ◽  
Carbon Nitride ◽  
Carbon Nitrides ◽  
Polymeric Carbon ◽  
Carbon Nitride Materials

The photocatalytic splitting of water into molecular hydrogen and molecular oxygen with sunlight is the dream reaction for solar energy conversion. Since decades, transition-metal-oxide semiconductors and supramolecular organometallic structures have been extensively explored as photocatalysts for solar water splitting. More recently, polymeric carbon nitride materials consisting of triazine or heptazine building blocks have attracted considerable attention as hydrogen-evolution photocatalysts. The mechanism of hydrogen evolution with polymeric carbon nitrides is discussed throughout the current literature in terms of the familiar concepts developed for photoelectrochemical water splitting with semiconductors since the 1970s. We discuss in this perspective an alternative mechanistic paradigm for photoinduced water splitting with carbon nitrides, which focusses on the specific features of the photochemistry of aromatic N-heterocycles in aqueous environments. It is shown that a water molecule which is hydrogen-bonded to an N-heterocycle can be decomposed into hydrogen and hydroxyl radicals by two simple sequential photochemical reactions. This concept is illustrated by first-principles calculations of excited-state reaction paths and their energy profiles for hydrogen-bonded complexes of pyridine, triazine and heptazine with a water molecule. It is shown that the excited-state hydrogen-transfer and hydrogen-detachment reactions are essentially barrierless, in sharp contrast to water oxidation in the electronic ground state, where high barriers prevail. We also discuss in some detail the products of possible reactions of the highly reactive hydroxyl radicals with the chromophores. We hypothesize that the challenge of efficient solar hydrogen generation with carbon-nitride materials is less the decomposition of water as such, but rather the controlled recombination of the photogenerated radicals to the closed-shell products H2 and H2O2.

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