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2024 Volume 43 Issue 12
2024, 43(12): 100414
doi: 10.1016/j.cjsc.2024.100414
Abstract:
In summary, atomically dispersed AuKPCN materials that can simultaneously promote the photocatalytic formation of ·OH and H2O2 have been developed, with apparent quantum efficiencies of more than 85% at 420 nm. Extensive experimental characterization and computa tional simulations have shown that the atomically dispersed Au with low oxidation number alters the band structure of the material to capture the highly localized holes created under light excitation. This study effectively overcomes the common challenge of slow kinetics of conventional 4e- WOR/2e- WOR process, and it is poised to serve as a significant milestone to inspire researchers in the field of photocatalytic water purification.
In summary, atomically dispersed AuKPCN materials that can simultaneously promote the photocatalytic formation of ·OH and H2O2 have been developed, with apparent quantum efficiencies of more than 85% at 420 nm. Extensive experimental characterization and computa tional simulations have shown that the atomically dispersed Au with low oxidation number alters the band structure of the material to capture the highly localized holes created under light excitation. This study effectively overcomes the common challenge of slow kinetics of conventional 4e- WOR/2e- WOR process, and it is poised to serve as a significant milestone to inspire researchers in the field of photocatalytic water purification.
2024, 43(12): 100398
doi: 10.1016/j.cjsc.2024.100398
Abstract:
In summary, for charge transfer kinetics, interfacial chemical bonds can reduce the energy barrier to promote charge separation and migra tion. Additionally, for the surface OER reaction, they can also activate reaction intermediates for lowing the overpotential to accelerate the reaction rate.
In summary, for charge transfer kinetics, interfacial chemical bonds can reduce the energy barrier to promote charge separation and migra tion. Additionally, for the surface OER reaction, they can also activate reaction intermediates for lowing the overpotential to accelerate the reaction rate.
2024, 43(12): 100427
doi: 10.1016/j.cjsc.2024.100427
Abstract:
The development of effective adsorbent materials for capturing organic dyes and iodine is crucial to reduce the environmental impact and ensure human health. In this context, a two-dimensional (2D) Co3-based metal-organic framework SDU-CP-7 (SDU = Shandong University, CP = coordination polymer) was rationally designed with 4-(4-carboxyphenyl)-1,2,4-triazole (Hcpt) and 2,4,6-tri(4-pyridinyl)-1,3,5-triazine (tpt) as organic linkers. The SDU-CP-7 was comprehensively characterized using single-crystal X-ray diffraction analysis, thermogravimetric analysis, Fourier transform infrared spectroscopy, Raman spectroscopy, powder X-ray diffraction analysis and UV-vis spectroscopy. Molecular docking was conducted to elucidate potential binding sites on SDU-CP-7 for effective interactions with RhB and ST. Featuring negatively charged surface and trigonal microporous channels, SDU-CP-7 exhibits excellent adsorption capacities for organic dyes (919.2 mg/g for Rhodamine B and 1565 mg/g for Safranine T) as well as iodine (563.0 mg/g in solution and 1100 mg/g in the vapor phase). The exceptional adsorption performance of SDU-CP-7 for cationic dyes can be ascribed to the electrostatic interaction facilitated by negatively charged zeta potential and the size-matching principle, whereas the pyridine active sites in channels significantly enhance the binding affinity for iodine. Moreover, SDU-CP-7 can serve as chromatographic column filters for the rapid adsorption and separation of dyes. The results demonstrate excellent selective adsorption performance of SDU-CP-7, highlighting its potential for environmental and industrial applications.
The development of effective adsorbent materials for capturing organic dyes and iodine is crucial to reduce the environmental impact and ensure human health. In this context, a two-dimensional (2D) Co3-based metal-organic framework SDU-CP-7 (SDU = Shandong University, CP = coordination polymer) was rationally designed with 4-(4-carboxyphenyl)-1,2,4-triazole (Hcpt) and 2,4,6-tri(4-pyridinyl)-1,3,5-triazine (tpt) as organic linkers. The SDU-CP-7 was comprehensively characterized using single-crystal X-ray diffraction analysis, thermogravimetric analysis, Fourier transform infrared spectroscopy, Raman spectroscopy, powder X-ray diffraction analysis and UV-vis spectroscopy. Molecular docking was conducted to elucidate potential binding sites on SDU-CP-7 for effective interactions with RhB and ST. Featuring negatively charged surface and trigonal microporous channels, SDU-CP-7 exhibits excellent adsorption capacities for organic dyes (919.2 mg/g for Rhodamine B and 1565 mg/g for Safranine T) as well as iodine (563.0 mg/g in solution and 1100 mg/g in the vapor phase). The exceptional adsorption performance of SDU-CP-7 for cationic dyes can be ascribed to the electrostatic interaction facilitated by negatively charged zeta potential and the size-matching principle, whereas the pyridine active sites in channels significantly enhance the binding affinity for iodine. Moreover, SDU-CP-7 can serve as chromatographic column filters for the rapid adsorption and separation of dyes. The results demonstrate excellent selective adsorption performance of SDU-CP-7, highlighting its potential for environmental and industrial applications.
2024, 43(12): 100453
doi: 10.1016/j.cjsc.2024.100453
Abstract:
Targeted electron transfer to catalytically active site for CO2 reduction is promising for enhancing the efficiency of artificial photosynthesis. Here, we demonstrate a design of an alkyl-linked heterostructure composing of TiO2 and a Cu-porphyrin-based covalent organic framework (TiO2@CuPorTT-COF) for the photoreduction of CO2 with H2O. Through specific coordination effect, the alkyl chain bridges TiO2 and Cu moiety in COF. Upon light illumination, the photoinduced electrons in TiO2 can be directionally transported across the interface along the alkyl chain to the Cu active sites to reduce adsorbed CO2, while the left holes are consumed by the H2O oxidation, enhancing the spatial separation and utilization of electron-hole pairs. Accordingly, the TiO2@CuPorTT-COF enables remarkably superior catalytic activities over the counterpart without the alkyl bridge for electron transfer with 5 times of CO production rate. An apparent quantum efficiency of 0.455% at 380 nm is achieved. Moreover, a dynamic evolution of Cu active site for CO2 reduction is revealed, which can be promoted by the targeting electron transport approach. This work provides a targeted electron transport strategy for constructing photocatalysts.
Targeted electron transfer to catalytically active site for CO2 reduction is promising for enhancing the efficiency of artificial photosynthesis. Here, we demonstrate a design of an alkyl-linked heterostructure composing of TiO2 and a Cu-porphyrin-based covalent organic framework (TiO2@CuPorTT-COF) for the photoreduction of CO2 with H2O. Through specific coordination effect, the alkyl chain bridges TiO2 and Cu moiety in COF. Upon light illumination, the photoinduced electrons in TiO2 can be directionally transported across the interface along the alkyl chain to the Cu active sites to reduce adsorbed CO2, while the left holes are consumed by the H2O oxidation, enhancing the spatial separation and utilization of electron-hole pairs. Accordingly, the TiO2@CuPorTT-COF enables remarkably superior catalytic activities over the counterpart without the alkyl bridge for electron transfer with 5 times of CO production rate. An apparent quantum efficiency of 0.455% at 380 nm is achieved. Moreover, a dynamic evolution of Cu active site for CO2 reduction is revealed, which can be promoted by the targeting electron transport approach. This work provides a targeted electron transport strategy for constructing photocatalysts.
2024, 43(12): 100457
doi: 10.1016/j.cjsc.2024.100457
Abstract:
The rapid decomposition of H2O2 on the surface of inorganic photocatalyst (BiVO4) and insufficient proton supply from water leads to a low photosynthetic yield of H2O2. Herein, hydrous tin dioxide (HSnO) with massive hydroxyl groups is coated on the BiVO4 surface to greatly improve the photocatalytic H2O2 activity via simultaneous realization of providing sufficient protons and inhibiting H2O2 decomposition. After coating HSnO, Au nanoparticles as the O2-reduction active sites are selectively deposited on the (010) facet of BiVO4 to synthesize Au/BiVO4@HSnO photocatalyst. The resulting Au/BiVO4@HSnO photocatalyst exhibits excellent H2O2-production performance, in which the photogenerated H2O2 concentration (210.7 μmol L-1) is about 4.8 times higher than that of Au/BiVO4 after 2 h light irradiation in pure water. The outstanding photocatalytic performance can be attributed to simultaneous enhancement of H2O2 generation and the suppression of H2O2 decomposition by HSnO coating. Specifically, the HSnO coating with massive hydroxyl groups provides enough protons to promote the catalytic transformation of O2 into H2O2 on Au nanoparticles. More importantly, this coating not only allows water molecules to effectively permeate onto BiVO4 surface for rapid oxidation reaction, but also greatly inhibits the reverse reaction of H2O2 decomposition via decreasing its affinity with BiVO4 surface. This research offers new insights for boosting photocatalytic H2O2 production through surface coating strategy.
The rapid decomposition of H2O2 on the surface of inorganic photocatalyst (BiVO4) and insufficient proton supply from water leads to a low photosynthetic yield of H2O2. Herein, hydrous tin dioxide (HSnO) with massive hydroxyl groups is coated on the BiVO4 surface to greatly improve the photocatalytic H2O2 activity via simultaneous realization of providing sufficient protons and inhibiting H2O2 decomposition. After coating HSnO, Au nanoparticles as the O2-reduction active sites are selectively deposited on the (010) facet of BiVO4 to synthesize Au/BiVO4@HSnO photocatalyst. The resulting Au/BiVO4@HSnO photocatalyst exhibits excellent H2O2-production performance, in which the photogenerated H2O2 concentration (210.7 μmol L-1) is about 4.8 times higher than that of Au/BiVO4 after 2 h light irradiation in pure water. The outstanding photocatalytic performance can be attributed to simultaneous enhancement of H2O2 generation and the suppression of H2O2 decomposition by HSnO coating. Specifically, the HSnO coating with massive hydroxyl groups provides enough protons to promote the catalytic transformation of O2 into H2O2 on Au nanoparticles. More importantly, this coating not only allows water molecules to effectively permeate onto BiVO4 surface for rapid oxidation reaction, but also greatly inhibits the reverse reaction of H2O2 decomposition via decreasing its affinity with BiVO4 surface. This research offers new insights for boosting photocatalytic H2O2 production through surface coating strategy.
2024, 43(12): 100458
doi: 10.1016/j.cjsc.2024.100458
Abstract:
The effective separation ability of photogenerated carriers plays a crucial role in catalytic hydrogen production. Establishing a heterojunction structure is an effective means to overcome the limited carrier separation ability of some single catalysts. In this paper, Cu, graphdiyne (GDY) and NiCoMoO4 are successfully coupled to construct a composite photocatalyst NCY-15%. The addition of sheet GDY effectively prevents the aggregation of NiCoMoO4, increases the number of active sites, and enhances the light-trapping ability of the composite catalyst. The synergistic interaction of S-scheme heterojunction and Ohmic junction heterojunction between Cu, GDY and NiCoMoO4 provides a unique transfer pathway for electrons, facilitating the rapid separation of photogenerated carriers and accelerating electron transfer, while retaining electrons with strong reducing capacity to participate in hydrogen production, thereby increasing the hydrogen evolution rate. This provides a new way for the development of GDY based photocatalysts.
The effective separation ability of photogenerated carriers plays a crucial role in catalytic hydrogen production. Establishing a heterojunction structure is an effective means to overcome the limited carrier separation ability of some single catalysts. In this paper, Cu, graphdiyne (GDY) and NiCoMoO4 are successfully coupled to construct a composite photocatalyst NCY-15%. The addition of sheet GDY effectively prevents the aggregation of NiCoMoO4, increases the number of active sites, and enhances the light-trapping ability of the composite catalyst. The synergistic interaction of S-scheme heterojunction and Ohmic junction heterojunction between Cu, GDY and NiCoMoO4 provides a unique transfer pathway for electrons, facilitating the rapid separation of photogenerated carriers and accelerating electron transfer, while retaining electrons with strong reducing capacity to participate in hydrogen production, thereby increasing the hydrogen evolution rate. This provides a new way for the development of GDY based photocatalysts.
2024, 43(12): 100462
doi: 10.1016/j.cjsc.2024.100462
Abstract:
Here, we report a novel visible-light-driven I- doped Bi2O2CO3 nano-sheet photocatalyst synthesized via a facile ion exchange route at room temperature. This obtained Bi2O2CO3 nano-sheet with I- doping shows several advantages. The specific surface area of I0.875-Bi2O2CO3 is 2.16 times higher than that of Bi2O2CO3, providing more catalytic sites for the degradation reactions. Moreover, a 3.2 times photocurrent enhancement is observed in I0.875-Bi2O2CO3 compared with Bi2O2CO3, producing more photogenerated electron-hole pairs for degradation. The synergistic effect between texture property and photoelectric effect boosts the removal of organic pollutants. Under visible light illumination, I0.875-Bi2O2CO3 displays superior photocatalytic performance for the degradation of methyl orange (MO) and phenol. Notably, a phenol degradation rate, 88%, is achieved by I0.875-Bi2O2CO3 with illuminating for 60 min, which is about 29 times higher than that of pristine Bi2O2CO3. This finding may provide an opportunity to develop a promising I- doped catalyst for organic pollutants removal.
Here, we report a novel visible-light-driven I- doped Bi2O2CO3 nano-sheet photocatalyst synthesized via a facile ion exchange route at room temperature. This obtained Bi2O2CO3 nano-sheet with I- doping shows several advantages. The specific surface area of I0.875-Bi2O2CO3 is 2.16 times higher than that of Bi2O2CO3, providing more catalytic sites for the degradation reactions. Moreover, a 3.2 times photocurrent enhancement is observed in I0.875-Bi2O2CO3 compared with Bi2O2CO3, producing more photogenerated electron-hole pairs for degradation. The synergistic effect between texture property and photoelectric effect boosts the removal of organic pollutants. Under visible light illumination, I0.875-Bi2O2CO3 displays superior photocatalytic performance for the degradation of methyl orange (MO) and phenol. Notably, a phenol degradation rate, 88%, is achieved by I0.875-Bi2O2CO3 with illuminating for 60 min, which is about 29 times higher than that of pristine Bi2O2CO3. This finding may provide an opportunity to develop a promising I- doped catalyst for organic pollutants removal.
2024, 43(12): 100463
doi: 10.1016/j.cjsc.2024.100463
Abstract:
Donor-π-acceptor (D-π-A) type photocatalysts with g-C3N4 as π-module have attracted much attention due to their optimized conjugate structure and enhanced electron directed driving. However, the inefficient charge migration of g-C3N4 due to its amorphous or semi-crystalline structure and limitation of available functional groups are present challenges. In this work, the D-π-A type high crystalline carbon nitride (HCCN) has been obtained by in-situ introducing amide and cyanide groups into the high-crystallinity melon framework. The synergistic effect of functional group modification and crystallinity regulation greatly enhances the electron induction driving and charge carrier density. Moreover, the density functional theory (DFT) calculations demonstrate that the D-π-A structure could induce the local charge distribution of melon units to provide a unique and stable pathway for photoinduced charge migration. The as-prepared HCCN sample shows a superior visible-light photocatalytic performance for hydrogen evolution with an apparent quantum efficiency (AQE) of 12.2% at 420 ± 15 nm, which is 23.7 times higher than that of original g-C3N4. Finally, the charge separation and transfer processes as well as the possible photocatalytic reaction mechanisms of HCCN sample are also investigated.
Donor-π-acceptor (D-π-A) type photocatalysts with g-C3N4 as π-module have attracted much attention due to their optimized conjugate structure and enhanced electron directed driving. However, the inefficient charge migration of g-C3N4 due to its amorphous or semi-crystalline structure and limitation of available functional groups are present challenges. In this work, the D-π-A type high crystalline carbon nitride (HCCN) has been obtained by in-situ introducing amide and cyanide groups into the high-crystallinity melon framework. The synergistic effect of functional group modification and crystallinity regulation greatly enhances the electron induction driving and charge carrier density. Moreover, the density functional theory (DFT) calculations demonstrate that the D-π-A structure could induce the local charge distribution of melon units to provide a unique and stable pathway for photoinduced charge migration. The as-prepared HCCN sample shows a superior visible-light photocatalytic performance for hydrogen evolution with an apparent quantum efficiency (AQE) of 12.2% at 420 ± 15 nm, which is 23.7 times higher than that of original g-C3N4. Finally, the charge separation and transfer processes as well as the possible photocatalytic reaction mechanisms of HCCN sample are also investigated.
2024, 43(12): 100472
doi: 10.1016/j.cjsc.2024.100472
Abstract:
Promoting efficient carrier separation and transfer can largely enhance photocatalytic performance and inhibit photo-corrosion. In this work, ZnCdS (ZCS) microspheres were obtained by a self-assembly strategy, and the Au/Co3O4/ZCS composites were synthesized by a modified photo-deposition method (loading Co3O4 and Au onto the surface of ZnCdS). The synergistic effect between the S-scheme heterojunction (Co3O4/ZCS) and Schottky junction (Au/ZCS) can effectively promote the generation and separation of photoelectrons and holes, thus enhancing the photocatalytic activity. Under visible light, the efficient photocatalysts showed hydrogen production activities up to 2525 μmol g-1 h-1, which is 2.24 times higher than that of Co3O4/ZCS and 6.92 times higher than that of pure ZnCdS. DFT calculations indicate that the built-in electric field between Co3O4/ZCS provides the driving force for efficient electron-hole separation, and the Au nanoparticles (NPs) act as electron collectors at the interface of ZnCdS to capture the electrons, which effectively prolongs the lifetime of photoelectrons and further enhances the photocatalytic hydrogen production activity.
Promoting efficient carrier separation and transfer can largely enhance photocatalytic performance and inhibit photo-corrosion. In this work, ZnCdS (ZCS) microspheres were obtained by a self-assembly strategy, and the Au/Co3O4/ZCS composites were synthesized by a modified photo-deposition method (loading Co3O4 and Au onto the surface of ZnCdS). The synergistic effect between the S-scheme heterojunction (Co3O4/ZCS) and Schottky junction (Au/ZCS) can effectively promote the generation and separation of photoelectrons and holes, thus enhancing the photocatalytic activity. Under visible light, the efficient photocatalysts showed hydrogen production activities up to 2525 μmol g-1 h-1, which is 2.24 times higher than that of Co3O4/ZCS and 6.92 times higher than that of pure ZnCdS. DFT calculations indicate that the built-in electric field between Co3O4/ZCS provides the driving force for efficient electron-hole separation, and the Au nanoparticles (NPs) act as electron collectors at the interface of ZnCdS to capture the electrons, which effectively prolongs the lifetime of photoelectrons and further enhances the photocatalytic hydrogen production activity.
2024, 43(12): 100473
doi: 10.1016/j.cjsc.2024.100473
Abstract:
Graphene quantum dots (GQDs) are a novel type of carbon dot material that has significant application value in the field of catalysis due to their non-toxic, stable, abundant surface functional groups, and quantum confinement effects. A unique composite photocatalyst was constructed by modifying GQDs onto Bi2MoO6 (BMO) microsphere-shaped nano petals using simple hydrothermal and sintering techniques. The structural and morphological characterization results indicate that GQDs with the size of 10 nm are well dispersed on BMO nanosheets, forming close contacts, which can greatly improve the separation efficiency of photo-generated electron-hole pairs under visible light irradiation. In the evaluation of the catalytic performance of BPA solution (20 mg/L) with a catalyst content of 20 mg under a simulated light source with a power of 300 W, the best degradation performance was achieved by a photocatalyst (G6/BMO) with the GQDs mass ratio of 6%, which degraded over 95% of BPA under visible light within 120 min, while pure BMO only degraded about 45% of BPA during the same time period. Even if the 400 nm filter is removed and directly exposed to Xe lamp radiation, the degradation performance of the optimal composite catalyst is only slightly improved, indicating that the current GQDs/BMO composite catalyst has extremely strong visible light catalytic activity. The improvement of catalytic performance comes from the effective separation of electron-hole pairs caused by the absorption of electrons by GQDs, and the introduction of GQDs to reduce the band gap and enhance visible light absorption, both of which are beneficial for catalytic reactions. Free radical capture and electron spin resonance (ESR) tests indicate that ·OH and ·O2- are the main active species for BPA degradation. Although the current GQDs/BMO catalysts have a simple structure, their catalytic performance has significantly improved, which will guide the design of other semiconductor based photocatalysts.
Graphene quantum dots (GQDs) are a novel type of carbon dot material that has significant application value in the field of catalysis due to their non-toxic, stable, abundant surface functional groups, and quantum confinement effects. A unique composite photocatalyst was constructed by modifying GQDs onto Bi2MoO6 (BMO) microsphere-shaped nano petals using simple hydrothermal and sintering techniques. The structural and morphological characterization results indicate that GQDs with the size of 10 nm are well dispersed on BMO nanosheets, forming close contacts, which can greatly improve the separation efficiency of photo-generated electron-hole pairs under visible light irradiation. In the evaluation of the catalytic performance of BPA solution (20 mg/L) with a catalyst content of 20 mg under a simulated light source with a power of 300 W, the best degradation performance was achieved by a photocatalyst (G6/BMO) with the GQDs mass ratio of 6%, which degraded over 95% of BPA under visible light within 120 min, while pure BMO only degraded about 45% of BPA during the same time period. Even if the 400 nm filter is removed and directly exposed to Xe lamp radiation, the degradation performance of the optimal composite catalyst is only slightly improved, indicating that the current GQDs/BMO composite catalyst has extremely strong visible light catalytic activity. The improvement of catalytic performance comes from the effective separation of electron-hole pairs caused by the absorption of electrons by GQDs, and the introduction of GQDs to reduce the band gap and enhance visible light absorption, both of which are beneficial for catalytic reactions. Free radical capture and electron spin resonance (ESR) tests indicate that ·OH and ·O2- are the main active species for BPA degradation. Although the current GQDs/BMO catalysts have a simple structure, their catalytic performance has significantly improved, which will guide the design of other semiconductor based photocatalysts.
2024, 43(12): 100474
doi: 10.1016/j.cjsc.2024.100474
Abstract:
Efficient separation and transfer of photogenerated carriers is one of the important factors for improving photocatalytic H2 production from water splitting. In this work, ZnIn2S4 nanosheets (NSs) with sulfur defect (Vs-ZIS) and TiO2 NSs with exposed {001} facets (001-TiO2 NSs) are fabricated firstly, then the novel 001-TiO2/Vs-ZIS heterojunction is constructed by employing NH4HCO3 as a binder, in which NH4+ attracts the 001-TiO2 and Vs-ZIS NSs to contact with each other and forms a compact 2D/2D heterostructure. Benefit from the suitable band structure of Vs-ZIS and 001-TiO2, the photoinduced electrons on 001-TiO2 recombine with the photoinduced holes on Vs-ZIS following Z-scheme mechanism, leading to the remarkable separation of photogenerated carriers. In addition, the synergistic effects of unique 2D/2D structure, highly active {001} facets and sulfur defect also contribute to the efficient separation of photogenerated carriers and enhanced photocatalytic activity in 001-TiO2/Vs-ZIS system. The obtained 2D/2D 001-TiO2/Vs-ZIS photocatalyst exhibits an outstanding H2 evolution rate of 17113 μmol g-1 h-1, which is approximately 1426- and 3-fold compared to those of 001-TiO2 NSs and Vs-ZIS NSs, respectively.
Efficient separation and transfer of photogenerated carriers is one of the important factors for improving photocatalytic H2 production from water splitting. In this work, ZnIn2S4 nanosheets (NSs) with sulfur defect (Vs-ZIS) and TiO2 NSs with exposed {001} facets (001-TiO2 NSs) are fabricated firstly, then the novel 001-TiO2/Vs-ZIS heterojunction is constructed by employing NH4HCO3 as a binder, in which NH4+ attracts the 001-TiO2 and Vs-ZIS NSs to contact with each other and forms a compact 2D/2D heterostructure. Benefit from the suitable band structure of Vs-ZIS and 001-TiO2, the photoinduced electrons on 001-TiO2 recombine with the photoinduced holes on Vs-ZIS following Z-scheme mechanism, leading to the remarkable separation of photogenerated carriers. In addition, the synergistic effects of unique 2D/2D structure, highly active {001} facets and sulfur defect also contribute to the efficient separation of photogenerated carriers and enhanced photocatalytic activity in 001-TiO2/Vs-ZIS system. The obtained 2D/2D 001-TiO2/Vs-ZIS photocatalyst exhibits an outstanding H2 evolution rate of 17113 μmol g-1 h-1, which is approximately 1426- and 3-fold compared to those of 001-TiO2 NSs and Vs-ZIS NSs, respectively.
2024, 43(12): 100466
doi: 10.1016/j.cjsc.2024.100466
Abstract:
Covalent organic frameworks (COFs) are a class of stable two- or three-dimensional porous materials which are composed of ordered organic units connected by strong covalent bonds. Owing to their outstanding physical and chemical properties, COFs have garnered significant attention in recent years as promising candidates for photocatalytic reduction of CO2. In this review, we will first summarize the synthesis and structures of COFs, then provide an overview of characterization techniques used for COFs, and finally systematically review recent research progress on the photocatalytic reduction of CO2 using COFs. Fully understanding of the relations between COFs structures and photocatalytic CO2 reduction would greatly enhance the further development of this emerging area. Herein we address this gap, aiming not only to provide the latest research progress of COFs materials in the photocatalytic reduction of CO2 but also to summarize the advanced characterizations for COFs structures and illustrate how the structures guide the photocatalytic reduction of CO2 performance.
Covalent organic frameworks (COFs) are a class of stable two- or three-dimensional porous materials which are composed of ordered organic units connected by strong covalent bonds. Owing to their outstanding physical and chemical properties, COFs have garnered significant attention in recent years as promising candidates for photocatalytic reduction of CO2. In this review, we will first summarize the synthesis and structures of COFs, then provide an overview of characterization techniques used for COFs, and finally systematically review recent research progress on the photocatalytic reduction of CO2 using COFs. Fully understanding of the relations between COFs structures and photocatalytic CO2 reduction would greatly enhance the further development of this emerging area. Herein we address this gap, aiming not only to provide the latest research progress of COFs materials in the photocatalytic reduction of CO2 but also to summarize the advanced characterizations for COFs structures and illustrate how the structures guide the photocatalytic reduction of CO2 performance.
2024, 43(12): 100469
doi: 10.1016/j.cjsc.2024.100469
Abstract:
g-C3N4 is a promising non-metallic photocatalyst recognized for its unique structural and physicochemical properties. Recent reviews have addressed g-C3N4-based photocatalysis; however, the rapid progress in big data and artificial intelligence has significantly accelerated the design, synthesis, and optimization of these materials. Machine learning, theoretical simulations, and advanced in-situ characterization techniques have deepened our understanding of their photocatalytic mechanisms. This review critically evaluates advancements in g-C3N4-based photocatalysts over the last two to three years, focusing on strategies to improve photogenerated charge separation, expand light absorption, and enhance stability and catalytic efficiency. It discusses cutting-edge in-situ characterization methods alongside machine learning approaches for predicting and optimizing applications in photocatalytic H2 evolution, CO2 reduction, pollutant degradation, H2O2 production, and nitrogen fixation. Finally, it proposes prospective strategies for further enhancing the performance of g-C3N4-based photocatalysts, aiming to guide the design of high-performance two-dimensional carbon-based photocatalysts.
g-C3N4 is a promising non-metallic photocatalyst recognized for its unique structural and physicochemical properties. Recent reviews have addressed g-C3N4-based photocatalysis; however, the rapid progress in big data and artificial intelligence has significantly accelerated the design, synthesis, and optimization of these materials. Machine learning, theoretical simulations, and advanced in-situ characterization techniques have deepened our understanding of their photocatalytic mechanisms. This review critically evaluates advancements in g-C3N4-based photocatalysts over the last two to three years, focusing on strategies to improve photogenerated charge separation, expand light absorption, and enhance stability and catalytic efficiency. It discusses cutting-edge in-situ characterization methods alongside machine learning approaches for predicting and optimizing applications in photocatalytic H2 evolution, CO2 reduction, pollutant degradation, H2O2 production, and nitrogen fixation. Finally, it proposes prospective strategies for further enhancing the performance of g-C3N4-based photocatalysts, aiming to guide the design of high-performance two-dimensional carbon-based photocatalysts.
