“…The bending of CN‐A nanosheets also creates a crumpled structure, leading to a much higher specific area. Importantly, the presence of C=O groups induces an upshift of the CB edge of CN‐A, which could thermodynamically promote the hydrogen evolution reaction . The subsequent calcination step in air produces more extraordinary features in CN‐AA.…”
Section: Resultsmentioning
confidence: 99%
“…Importantly,t he presence of C=Og roups induces an upshift of the CB edge of CN-A, which could thermodynamically promotet he hydrogen evolutionr eaction. [29] The subsequent calcination step in air produces more extraordinary features in CN-AA.S everalc arbon species in the CN-A framework were removed owing to the reaction with oxygen in air,c reatinga large number of in-plane nanoholes. The introduction of these nanoholes increased the specific surface area of CN-AA up to 270 m 2 g À1 ,w hich is one of the highest specific surfacea reas observed in carbon nitride materials.…”
Section: Thermal Polycondensation Of Mcs To Carbon Nitridenanosheets mentioning
A highly condensed lamellar melamine–cyanuric acid supramolecular (MCS) complex was synthesized in an autoclave at high pressure as a precursor for preparing g‐C3N4 nanosheets. Given the distinctive properties of the prepared MCS complex, an efficient g‐C3N4 nanosheet photocatalyst can be obtained by heat treatment of this MCS complex under Ar followed by calcination in air at 400 °C. The resulting nanosheets with in‐plane nanoholes showed an extremely high specific surface area (≈270 m2 g−1) and significantly enhanced light absorption in the visible region. This phenomenon is observed for the first time in carbon nitride nanosheets. The enhanced light absorption results from the sizeable conjugated system of tri‐striazine units in the carbon nitride framework, coupled with the structural defects arising from the presence of oxygen‐containing groups induced during the synthesis. Consequently, the obtained carbon nitride nanosheets exhibited excellent performance for hydrogen generation under sunlight and especially under visible light. Its quantum efficiency (QE) of 20.9 % at 420 nm is one of the highest reported values for carbon nitride materials. A QE of 3.5 % could be observed even at 590 nm. The integrated QE of this material in the visible region (420–600 nm) is approximately 1 %. To the best of our knowledge this is the highest value compared to all other the carbon nitride nanosheet materials reported previously.
“…The bending of CN‐A nanosheets also creates a crumpled structure, leading to a much higher specific area. Importantly, the presence of C=O groups induces an upshift of the CB edge of CN‐A, which could thermodynamically promote the hydrogen evolution reaction . The subsequent calcination step in air produces more extraordinary features in CN‐AA.…”
Section: Resultsmentioning
confidence: 99%
“…Importantly,t he presence of C=Og roups induces an upshift of the CB edge of CN-A, which could thermodynamically promotet he hydrogen evolutionr eaction. [29] The subsequent calcination step in air produces more extraordinary features in CN-AA.S everalc arbon species in the CN-A framework were removed owing to the reaction with oxygen in air,c reatinga large number of in-plane nanoholes. The introduction of these nanoholes increased the specific surface area of CN-AA up to 270 m 2 g À1 ,w hich is one of the highest specific surfacea reas observed in carbon nitride materials.…”
Section: Thermal Polycondensation Of Mcs To Carbon Nitridenanosheets mentioning
A highly condensed lamellar melamine–cyanuric acid supramolecular (MCS) complex was synthesized in an autoclave at high pressure as a precursor for preparing g‐C3N4 nanosheets. Given the distinctive properties of the prepared MCS complex, an efficient g‐C3N4 nanosheet photocatalyst can be obtained by heat treatment of this MCS complex under Ar followed by calcination in air at 400 °C. The resulting nanosheets with in‐plane nanoholes showed an extremely high specific surface area (≈270 m2 g−1) and significantly enhanced light absorption in the visible region. This phenomenon is observed for the first time in carbon nitride nanosheets. The enhanced light absorption results from the sizeable conjugated system of tri‐striazine units in the carbon nitride framework, coupled with the structural defects arising from the presence of oxygen‐containing groups induced during the synthesis. Consequently, the obtained carbon nitride nanosheets exhibited excellent performance for hydrogen generation under sunlight and especially under visible light. Its quantum efficiency (QE) of 20.9 % at 420 nm is one of the highest reported values for carbon nitride materials. A QE of 3.5 % could be observed even at 590 nm. The integrated QE of this material in the visible region (420–600 nm) is approximately 1 %. To the best of our knowledge this is the highest value compared to all other the carbon nitride nanosheet materials reported previously.
“…N/O‐doped carbonaceous photocatalysts (Table ) are prepared through thermal condensation of N ‐containing precursor in the presence of H 2 O 2 , the chemical oxidation post‐treatment of as‐prepared g‐C 3 N 4 by H 2 O 2 , or mixed acids (HNO 3 /H 2 SO 4 ), the photo Fenton reaction of g‐C 3 N 4 nanosheets by UV irradiation in the presence of Fe 2+ /Fe 3+ and H 2 O 2 , the heating post‐treatment of GO in NH 3 , or through a slicating approach of GO with 2D carbon nitride nanodots. Generally, the co‐doped carbonaceous photocatalysts show higher S BET , promoted light absorption, and prolonged lifetime of photogenerated electron‐hole pairs in different degrees, which are dependent on the doping method and doping level.…”
“…From Table , O, N ‐codoped carbonaceous photocatalysts have been used in hydrogen generation from water splitting, and the environmental purification by degradation of organic pollutants like RhB, MO, MB, phenol . Through O‐doping with appropriate content, distribution, and chemical state, the porous g‐C 3 N 4 photocatalysts with higher S BET , and the promoted light absorption as well as enhanced separation, transfer and recombination of photogenerated charge carriers can be ontained, which endows them with remarkably improved photocatalytic properties in contrast to pristine g‐C 3 N 4 .…”
“…N/O-doped carbonaceousphotocatalysts ( Table 7) are prepared through thermalc ondensation of N-containing precursor in the presence of H 2 O 2 , [264] the chemical oxidation post-treatment of as-prepared g-C 3 N 4 by H 2 O 2 , [265,266] or mixed acids (HNO 3 /H 2 SO 4 ), [267] the photo Fentonr eactiono fg -C 3 N 4 nanosheets by UV irradiation in the presence of Fe 2 + /Fe 3 + and H 2 O 2 , [177] the heating post-treatment of GO in NH 3 , [268] or throughas licatinga pproach [201] of GO with 2D carbon nitride nanodots.G enerally,t he co-doped carbonaceousp hotocata- ( Figure 22 b, c), shows 4.4 times higher S BET with 0.09 cm 3 g À1 of V total and 20.7 nm of pore size, narrower band gap by 0.08 eV,m uch lower PL intensity and significantly promoted conductivity than pristine g-C 3 N 4 (Figure 22 d, e). By increasing Oc ontent from 1.5 to 3.0 at %, the as-preparedM CN-2 features similar morphology, S BET ,a nd V total to MCN-1, but it exhibits 39.3 nm of larger pore size and the 150 nm of larger cavity size.…”
Section: Nitrogen and Oxygend Ual-doped Carbonaceousp Hotocatalystsmentioning
Photocatalytic solar energy conversion and environmental remediation including water splitting, CO2 reduction, and pollutant degradation have attracted rapidly growing attention, owing to global fossil fuel depletion and increasing environmental issues. From the viewpoint of the broad availability, good environmental acceptability, high corrosion resistance, as well as the readily tailorable microstructure, electronic structure and surface chemical properties, carbonaceous materials have been demonstrated as promising and sustainable low‐cost metal‐free alternatives to metal‐based photocatalysts for solar fuel production and pollutant degradation. The non‐metallic heteroatoms doping approach has been considered as a powerful tool for modulating electronic structure, morphology, surface structure and surface chemistry, textural properties, optical properties, and electrochemical properties, as well as catalytic properties of carbonaceous photocatalysts. This Review represents a comprehensive overview of the latest advance in preparation and physicochemical properties of diverse non‐metallic heteroatoms‐doped carbonaceous materials, as well as their applications in heterogeneous photocatalysis towards solar energy conversion and environmental remediation. The physicochemical properties and photocatalytic performance of the carbonaceous photocatalysts are carefully compared, as well as a brief overview of fundamental principles for the promoting effect of heteroatoms‐doping is also presented. In addition, the future perspectives on the opportunities and challenges of heteroatoms doping for fabricating novel and excellent carbonaceous photocatalysts are outlined.
Photo(electro)catalytic nitrogen fixation is considered as a competing alternative for the Haber–Bosch (HB) process due to the direct production of ammonia (NH3) from nitrogen and water with zero carbon dioxide emission, which has made it a very hot research topic in recent years. Particularly, photo‐driven nitrogen reduction has been attracted to a specific focus in the scientific community since it can be powered by limitless solar energy at ambient conditions. However, unsolved challenges have remained to date such as, electron–hole separation, low quantum efficiency, weak visible light harvesting, catalytic selectivity, N2 adsorption, and activation. In this Review, the recent achievements and related approaches toward nitrogen fixation are presented. In addition, the discussions on mechanistic photofixation of nitrogen, catalytic engineering design, and the outlook for enhancing the photocatalytic performance of ammonia photosynthesis are also devoted. Finally, the emerging trend of advanced photo(electro)catalysts for nitrogen fixation is proposed.
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