Enhancing photocatalytic hydrogen production of carbon nitride: Dominant advantage of crystallinity over mass transfer
Shuling WangFengting HeYang‐Ming LuYuzhao WuYang ZhangPei DongXiaoming LiuChaocheng ZhaoShuaijun WangDejun WangJinqiang ZhangShaobin Wang
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Abstract:
Mass transfer enhancement and crystallinity engineering are two prevailing technologies for photocatalyst modification. However, their relative effectiveness in enhancing photocatalytic activity remains unclear due to the lack of rational probing catalysts. In this study, we synthesized two distinct carbon nitride (C3N4) catalysts: one with a high specific surface area (CN-HA) and the other with improved crystallinity (CN-HC). These catalysts served as probes to compare their respective impacts on photocatalytic activities. Comprehensive characterization techniques and density functional theory (DFT) calculation results unveiled that crystallinity played a dominant role in light absorption and charge dynamics, while surface area primarily influenced mass transfer in photocatalysis. Importantly, our findings revealed that crystallinity engineering of photocatalyst achieved a greater impact on photocatalytic hydrogen evolution than that from mass transfer enhancement. Consequently, CN-HC demonstrated a remarkable improvement in photocatalytic performance for hydrogen evolution (6465.4 μmol h-1 g-1), surpassing both C3N4 and CN-HA by 19.4- and 2.4-fold, respectively, accompanied by a high apparent quantum yield of 23.8 % at 420 nm. This study not only unveils the dominant factor influencing the activity of photocatalysts but also provides a modified approach for robust solar fuel production, shedding light on the path toward efficient and sustainable energy conversion.Keywords:
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Graphitic carbon nitride materials show some promising properties for applications such as photocatalytic water splitting. However, the conversion efficiency is still low due to factors such as a low surface area and limited light absorption. In this paper, we describe a “triple templating” approach to generating porous graphitic carbon nitride. The introduction of pores on several length-scales results in enhanced photocatalytic properties.
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The MoS2/S-doped graphitic carbon nitride (MoS2/S-g-C3N4) was synthesized by a simple method and applied for methylene blue (MB) removal as an organic pollutant. The structure of MoS2/S-doped graphitic carbon nitride was characterized using FTIR, XRD, SEM, TGA and BET techniques. The accomplishment of MoS2/S-doped graphitic carbon nitride as an adsorbent was investigated to removal of MB from aqueous solution. The various parameters were studied such as: pH, initial MB concentration, adsorbent dose, temperature and time. The best findings were obtained at pH=8, 8 ppm MB concentration, 0.05 g MoS2/S-g-C3N4, 30 min and 22 ˚C. The Langmuir isotherm model was adopted with the obtained data. The kinetic studies were showed that the adsorption of methylene blue can be well described by the second-order equation. Maximum adsorption was calculated as 166 mg/g. The degradation of MB was studied by MoS2/S-doped graphitic carbon nitride under Light Emmition Diode (LED). Results showed that the MoS2/S-doped graphitic carbon nitride can enhance photocatalytic activity compared to pure g-C3N4 and MoS2/g-C3N4. The findings confirmed that the MoS2/S-doped graphitic carbon nitride can be applied as an efficient, low-cost adsorbent, and photocatalyst to remove of cationic dyes such as methylene blue.
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In this article we report on the one-step, rapid, high-yield synthesis of graphitic carbon nitride (g-C3N4) nanosheets for the first time. The nanosheets were obtained by pyrolyzing a melamine–KBH4 mixture under Ar. As a fluorosensor for Cu2+, the g-C3N4 nanosheets exhibit a detection limit as low as 0.5 nM and high selectivity in buffer solutions, and this sensor was applied to the analysis of lake water samples. The electrogenerated chemiluminescence (ECL) behavior of the g-C3N4 nanosheets using Na2S2O8 as the coreactant was also studied. Results suggest that the ECL intensity of the g-C3N4 nanosheets was linear over concentrations of 0–45 nM, with a detection limit of 1.2 nM for Cu2+.
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The combination of cobalt redox catalysis and carbon nitride photocatalysis to construct a cascade photoreaction system has been developed for the deoxygenative reduction of CO2 to CO with visible light. The graphitic carbon nitride has been demonstrated to function both as a capture/activation substrate of CO2 and a photocatalyst, whereas the introduced cobalt species act as reductive and oxidative promoters to accelerate charge-carrier separation and transfer kinetics. This hybrid photosystem contains inexpensive substances that synergetically catalyze CO2-to-CO conversion at mild conditions, with a high stability of catalysts. The optimization in the surface and texture structures as well as reaction conditions has been demonstrated. The results represent an important step toward artificial photosynthesis by using cost-acceptable materials.
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We demonstrate that graphitic carbon nitride can photoreduce CO2 to CO in the presence of water vapor and exhibit interesting porous structure dependent reactivity on photoreduction and photooxidation under visible light (λ > 420 nm). Graphitic carbon nitride was synthesized by directly heating the inexpensive melamine and the replacement of melamine with melamine hydrochloride could result in porousification in the final graphitic carbon nitride with much higher surface area (39 times) and more abundant pores, accompanied by a band gap increase of 0.13 eV. The porousification could significantly enhance the photoreactivity of graphitic carbon nitride in rhodamine B photooxidation by 9.4 times, but lower its activity in CO2 photoreduction by 4.6 times. The reasons for the porous structure dependent photoreactivity were investigated in detail. These new findings could shed light on the design of efficient photocatalysts and the tuning of their photoreactivity for environmental and energy applications.
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