DFT Study on Sulfur-Doped g-C3N4 Nanosheets as a Photocatalyst for CO2 Reduction Reaction

Wang, Yuelin; Tian, Yu; Yan, Likai; Su, Zhong‐Min

doi:10.1021/acs.jpcc.8b00098

Cited by 223 publications

(133 citation statements)

References 51 publications

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“…The formation energies ( E form ) of different doped systems were calculated to evaluate the stability of different doped models, where E form was calculated using Equation :

true E_{form} = E_{doped} - E_{undoped} - μ_{P} + μ_{X}

…”

Section: Methodsmentioning

confidence: 99%

Phosphorus‐Functionalized Fe₂VO₄/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

et al. 2020

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The binary transition metal oxides have attracted great attention because of their considerable energy and power densities. However, they suffer from low reaction kinetics and large volume change, limiting their practical energy applications. The construction of a mesoporous structure with a large surface area, the development of a carbon matrix, as well as heteroatom doping can effectively overcome the above challenges. Herein, the synthesis of phosphorous‐containing Fe2VO4/nitrogen‐doped carbon mesoporous nanowires (P‐Fe2VO4/NCMNWs) is reported. In this unique structure, the atomic‐level P‐doping could increase the conductivity of Fe2VO4 by reducing its band gap, which is confirmed by DFT calculations. Furthermore, the phosphorus can covalently “bridge” the carbon layer and Fe2VO4 through P−C and Fe−O−P bondings. As a result, this anode material exhibits a high capacity (1002 mA h g−1 at 0.5 A g−1 after 250 cycles), excellent rate performance (448 mA h g−1 at 10 A g−1), and prominent long‐term cycling stability (533 mA h g−1 at 5 A g−1 after 500 cycles, 364 mA h g−1 at 10 A g−1 after 1000 cycles). All of these attractive features make the P‐Fe2VO4/NCMNWs a promising electrode material for high‐performance lithium‐ion batteries.

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“…The formation energies ( E form ) of different doped systems were calculated to evaluate the stability of different doped models, where E form was calculated using Equation :

true E_{form} = E_{doped} - E_{undoped} - μ_{P} + μ_{X}

…”

Section: Methodsmentioning

confidence: 99%

Phosphorus‐Functionalized Fe₂VO₄/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

et al. 2020

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“…[ [34][35][36] 3.3.2 | Kinetics Figure S1 shows the transition state structures of all steps. Kinetic studies of the first step show that the C-H bond distances in the reactant, TS1…”

Section: Thermodynamicsmentioning

confidence: 99%

“…COOH) is 1.15 eV. [36] Considering the advantages of the P-doped g-C 3 N 4 for the reduction of CO 2 , in this work, P-doped g-C 3 N 4 was synthesized and characterized by different techniques. The structure and electronic properties were investigated by using the SIESTA code.…”

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confidence: 99%

P‐doped g‐C₃N₄ as an efficient photocatalyst for CO₂ conversion into value‐added materials: a joint experimental and theoretical study

Ranjbakhsh

Izadyar

Nakhaeipour

et al. 2020

Int J of Quantum Chemistry

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The photocatalytic yield of g-C 3 N 4 for CO 2 reduction was modified by phosphorus doping. Possible reaction pathways for CO 2 reduction on the P-doped g-C 3 N 4 (PCN) surface were investigated by density function theory calculations for the first time. The experimental results showed that P doping increases the carriers' lifetime, which improves the production of CH 4 through the increase in the driving force of the electrons. The partial density of states of the PCN showed that the valence band maximum and conduction band minimum are composed of p x , p y , and, s orbitals of the N atoms and p z states of carbon, nitrogen, and phosphorus, respectively. Mechanism studies confirm that formic acid, formaldehyde, methanol, and methane are the most probable products. Methane, having positive adsorption energy, can be easily desorbed from the PCN surface, and the Gibbs activation energy of the final step is 1.98 eV. The formation of H 2 COOH is the rate-determining step. K E Y W O R D S adsorption, CO 2 reduction, g-C 3 N 4 , P-doped, photocatalyst 1 | INTRODUCTION The rise in the concentration of atmospheric carbon dioxide due to the continuous use of fossil fuels by humans has led to global warming. [1] In recent years, the efforts for the decrease in the CO 2 concentration have attracted great interest. However, CO 2 is a stable molecule from the thermodynamic and kinetic aspects that makes it difficult to convert CO 2 into valuable chemicals and fuels. [2] Inspired by photosynthesis in plants, the photocatalytic reduction of CO 2 into formic acid (HCOOH), formaldehyde (HCHO), methanol (CH 3 OH), methane (CH 4), and other chemicals and fuels was investigated by using TiO 2 , CuO/Cu 2 O, fullerene, ZnS, porous organic frameworks (POF), heterogeneous catalysts, and graphitic carbon nitrides. [3-9] Graphitic carbon nitride (g-C 3 N 4) is a metal-free polymeric semiconductor that has unique properties, such as nontoxicity; biocompatibility; high thermal and chemical stability [10-12] ; visible wavelength absorption; and also the position of the suitable conductive band (CB) (−1.23 V vs NHE) for reduction of CO 2 to HCOOH (−0.61 V), CO (−0.53 V), HCHO (−0.48 V), CH 3 OH (−0.38 V), and CH 4 (−0.24 V). [12-14] However, the photocatalytic efficiency of the g-C 3 N 4 is relatively low, owing to the fast recombination of the electron-hole pair and weak visible lightharvesting ability. [15] To overcome these drawbacks, several modification methods were applied, including doping with metal and nonmetal elements, [9,16-18] modification of the morphology [19]), construction of type-II and Z-scheme heterojunction, and cocatalyst loading. [20-22] Among these methods, nonmetal doping reduces the band gap and subsequently increases the photocatalytic efficiency. Furthermore, the CB and VB edge positions are suitable for photocatalytic reactions, and metal-free properties of the g-C 3 N 4 are still maintained. Theoretical and experimental investigations show that doped-g-C 3 N 4 by O, P, and S atoms increase the photocatalytic effi...

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“…Doping with non-metal impurities narrows the band gap of the g-C 3 N 4 and stimulates its photocatalytic performance [25]. In particularly, S atoms can substitute for the N atoms of g-C 3 N 4 due to suitable electronegativity and ionic radius, consequently leading to more favorable redox properties for enhanced photocatalytic activity [26]. Liu et al [27] synthesized S-doped g-C 3 N 4 from as-synthesized g-C 3 N 4 powder calcined at 450 °C under a high-purity H 2 S gaseous atmosphere.…”

Section: Introductionmentioning

confidence: 99%

Dual Functional S-Doped g-C3N4 Pinhole Porous Nanosheets for Selective Fluorescence Sensing of Ag+ and Visible-Light Photocatalysis of Dyes

2019

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This study explores the facile, template-free synthesis of S-doped g-C3N4 pinhole nanosheets (SCNPNS) with porous structure for fluorescence sensing of Ag+ ions and visible-light photocatalysis of dyes. As-synthesized SCNPNS samples were characterized by various analytical tools such as XRD, FT-IR, TEM, BET, XPS, and UV–vis spectroscopy. At optimal conditions, the detection linear range for Ag+ was found to be from 0 to 1000 nM, showing the limit of detection (LOD) of 57 nM. The SCNPNS exhibited highly sensitive and selective detection of Ag+ due to a significant fluorescence quenching via photo-induced electron transfer through Ag+–SCNPNS complex. Moreover, the SCNPNS exhibited 90% degradation for cationic methylene blue (MB) dye within 180 min under visible light. The enhanced photocatalytic activity of the SCNPNS was attributed to its negative zeta potential for electrostatic interaction with cationic dyes, and the pinhole porous structure can provide more active sites which can induce faster transport of the charge carrier over the surface. Our SCNPNS is proposed as an environmental safety tool due to several advantages, such as low cost, facile preparation, selective recognition of Ag+ ions, and efficient photocatalytic degradation of cationic dyes under visible light.

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DFT Study on Sulfur-Doped g-C₃N₄ Nanosheets as a Photocatalyst for CO₂ Reduction Reaction

Cited by 223 publications

References 51 publications

Phosphorus‐Functionalized Fe₂VO₄/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

Phosphorus‐Functionalized Fe₂VO₄/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

P‐doped g‐C₃N₄ as an efficient photocatalyst for CO₂ conversion into value‐added materials: a joint experimental and theoretical study

Dual Functional S-Doped g-C3N4 Pinhole Porous Nanosheets for Selective Fluorescence Sensing of Ag+ and Visible-Light Photocatalysis of Dyes

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DFT Study on Sulfur-Doped g-C3N4 Nanosheets as a Photocatalyst for CO2 Reduction Reaction

Cited by 223 publications

References 51 publications

Phosphorus‐Functionalized Fe2VO4/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

Phosphorus‐Functionalized Fe2VO4/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

P‐doped g‐C3N4 as an efficient photocatalyst for CO2 conversion into value‐added materials: a joint experimental and theoretical study

Dual Functional S-Doped g-C3N4 Pinhole Porous Nanosheets for Selective Fluorescence Sensing of Ag+ and Visible-Light Photocatalysis of Dyes

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DFT Study on Sulfur-Doped g-C₃N₄ Nanosheets as a Photocatalyst for CO₂ Reduction Reaction

Phosphorus‐Functionalized Fe₂VO₄/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

Phosphorus‐Functionalized Fe₂VO₄/Nitrogen‐Doped Carbon Mesoporous Nanowires with Exceptional Lithium Storage Performance

P‐doped g‐C₃N₄ as an efficient photocatalyst for CO₂ conversion into value‐added materials: a joint experimental and theoretical study