INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Yijun Luo,Wenxin Yang,Jincheng Liu,Wei Cai,Zewei Liao,Xiaoyan Xiang,Bingjie Li,Yanxiong Fang
The concurrent production of renewable hydrogen and valorization of biomass represents a promising strategy to tackle energy sustainability and environmental concerns. However, designing efficient bifunctional photocatalytic systems capable of driving both reactions remains a significant challenge. This study introduces a Z-scheme heterojunction composed of graphitic carbon nitride (g-C 3 N 4 ) and titanium dioxide (TiO 2 ), synthesized through a combined hydrothermal and self-assembly approach, for simultaneous photocatalytic H 2 evolution and selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF). The heterostructure establishes an internal electric field that directs photogenerated electrons to g-C 3 N 4 and holes to TiO 2 , thereby facilitating effective charge-carrier separation while preserving their strong redox potentials . Structural analyses confirm the uniform growth of TiO 2 nanorods with reduced diameter of less than 10 nm on g-C 3 N 4 nanosheets, which enhances light harvesting and exposes abundant reactive sites. Under optimized conditions, the composite exhibited exceptional performance, achieving H 2 and DFF production rates of 481.9 μmol g −1 h −1 , respectively, with 92.8 % DFF selectivity. This represents a 3.8-fold enhancement in activity compared to pristine g-C 3 N 4 . The improved efficiency is attributed to the Z-scheme charge-transfer pathway, which mitigates recombination losses and optimizes the utilization of electrons and holes for respective reduction and oxidation reactions. This work provides a scalable framework for integrating green hydrogen generation with biomass refining, advancing the development of multifunctional photocatalysts for sustainable energy and chemical synthesis.
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Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Tieliang Bai,Wei Chen,Runqing Zhang,Fuhao Yin,Mao Xu,Benxia Li
Coupling O 2 reduction and selective organic oxidation for photocatalytic coproduction of H 2 O 2 and value-added organic compounds (e.g., benzaldehyde) represents a dual-functional strategy to maximize solar energy utilization and economic benefits in chemical manufacturing. Employing water/organic biphasic systems for such reactions offers a sustainable solution to address the challenges inherent in conventional single-phase systems, such as energy-intensive product separation and uncontrolled secondary reactions. Herein, we rationally designed and synthesized an amphiphilic BiOBr/g-C 3 N 4 S-scheme heterojunction photocatalyst (labeled as BOB/PCN-A) composed of hierarchically structured BiOBr and porous g-C 3 N 4 , which can stably localize at the water/toluene biphasic interface. This unique feature enables the formation of a quasi-Pickering emulsion under continuous stirring during the photocatalytic process, facilitating the simultaneous production and in situ separation of H 2 O 2 in the aqueous phase and benzaldehyde in the organic phase. The S-scheme heterojunction enhances visible-light absorption, promotes efficient electron-hole separation, and preserves the strong redox potential of photogenerated charge carriers. Under simulated sunlight, the optimized BOB/PCN-A photocatalyst achieves remarkable production rates of 2.29 mmol g −1 h −1 for benzaldehyde and 1.77 mmol g −1 h −1 for H 2 O 2 , with a 100 % selectivity toward benzaldehyde. This study showcases a green photocatalytic system that integrates synthesis and separation processes, offering promising implications for sustainable solar-driven chemical manufacturing.
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LANGMUIR
·
2025
·
IF 3.9
Dan Wang,Qiang Le,Wang Zhang,Zhaodong Nan
Carbon nitride (g-C3N4, CN) is always used as a metal-free catalyst to activate peroxymonosulfate (PMS) without toxic metal ion leaching in solutions. However, it is still a challenge to enhance the catalytic activity for CN. Herein, sulfur (S)-doped g-C3N4 is synthesized by a facile method as named CNSx, where x represents the mass ratio of ammonium sulfate to melamine during the CNSx synthesis. Partial N atoms such as pyridinic N in CN were replaced by S atoms. CNS1.75 exhibited an excellent catalytic activity to degrade Rhodamine B (RhB) via PMS activation under the assistance of the visible light (Vis). The rate constant (k) increased about 9 and 7 times for CNS1.75/Vis/PMS than that of CNS1.75/PMS and CNS/Vis/PMS systems. Moreover, the k value is higher than that of some metal-doped CN as reported. The toxicity of RhB was effectively reduced after the degradation process with the total organic carbon (TOC) removal ratio 48% after 40 min. The RhB removal efficiency kept 95% after continuous operation for 12 h. The catalytic mechanism was proposed in which 1O2 was the dominant reactive oxygen species (ROS).
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Kexin Yang,Zhijia Song,XiaoXiao Fu,Wei Yan,Tao Zhang,Yiwei Hua,Haixin Lin,Qin Kuang,Zhaoxiong Xie
The photocatalytic direct one-step two-electron (2e-) oxygen reduction reaction (ORR) holds great potential in efficient H2O2 synthesis. However, it is still a significant challenge to design photocatalysts for achieving high-efficiency H2O2 production via this direct one-step 2e- ORR pathway. To address this, we have constructed a Z-scheme BAIO/C3N4 heterojunction by in situ growing Ba2AgIO6 (BAIO) on the surface of C3N4 nanosheets. Under visible light irradiation, the optimal sample, with a BAIO:C3N4 mass ratio of 1:1.5, exhibited a remarkable H2O2 yield of up to 535.9 μmol g-1 h-1, which is 8.8 times higher than that of pure C3N4. This enhancement is attributed to the improved charge separation and migration efficiency facilitated by the enhanced internal electric field (IEF) in BAIO/C3N4 heterojunction. Furthermore, the heterojunction altered the O2 adsorption configuration to the Yeager-type, promoting a more efficient and selective direct one-step 2e- ORR for H2O2 production. This study highlights the importance of regulating the reaction pathway to enhance photocatalytic H2O2 production activity and offers a new insight for designing highly active photocatalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Qin Jiao,Binchuan Gao,Li Zhang,Ruijie Chen,Lei Wang,Qiang Wang,Nengjie Feng,Hui Wan,Guofeng Guan,Mingjuan Han
The photocatalytic performance of graphitic carbon nitride (g-C 3 N 4 ) in the conversion of CO 2 to CH 3 OH is intrinsically constrained by its limited selectivity and activity. Herein, we developed a dual-modification strategy that integrates S doping into the g-C 3 N 4 (CN) skeleton and constructed a 2D/2D S-doped g-C 3 N 4 /Bi 2 MoO 6 Z-scheme heterojunction (SCN/BMO) via microwave-assisted synthesis. This strategy achieved sulfur doping through N-site substitution to modulate the electronic structure of CN, resulting in the formation of a 2D/2D SCN/BMO Z-scheme heterojunction. The optimized 0.3SCN/BMO photocatalyst achieved a methanol production rate of 6.19 μmol·g −1 ·h −1 with 99.15 % selectivity under solar irradiation, showing a 5.16-fold and 2.60-fold enhancement in catalytic activity compared to pristine g-C 3 N 4 and Bi 2 MoO 6 (BMO), respectively. Meanwhile, it demonstrated excellent photocatalytic and structural stability during the cycling tests. Systematic characterization analyses have revealed that the synergistic light-harvesting effect, optimized interfacial coupling, and efficient charge transport pathways within the 2D/2D 0.3SCN/BMO Z-scheme heterostructure collectively contribute to the significant enhancement in photocatalytic performance. Moreover, a feasible photocatalytic mechanism has been put forward by combining the outcomes of in-situ DRIFT spectroscopic analysis with DFT computational modeling. This research finding provides an innovative strategy for the development of highly efficient photocatalysts, which are specifically designed for the selective reduction conversion of CO 2 to CH 3 OH.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Dingzhou Xiang,Shiqi Zhang,Guanghui Cheng,Lu Li,Xing Wang,Chenghuan Zhong,Shan Gao
Direct photocatalytic methane conversion into high-value liquid oxygenates has garnered significant research interest under mild conditions, yet a critical challenge is to obtain an excellent formaldehyde yield rate and selectivity only using H 2 O as the oxidant. Herein, a 2D g-C 3 N 4 nanosheet/ 0D ZnO quantum dots (ZCN) Z -scheme heterojunction was established by the self-assembly strategy to acquire an outstanding C1 liquid oxygenates (methanol and formaldehyde) with productivity of 908.13 μmol g cat −1 h −1 under ambient temperature and pressure without extra oxidant. Notably, the HCHO yield rate could be reached to 706.32 μmol g cat −1 h −1 with a selectivity of 69 %. The confinement effect of ZnO quantum dots (ZnO QDs) broadens the bandgap to some extent, making the catalyst possess a strong oxidation potential that could oxidize H 2 O to generate enough hydroxyl radical ( · OH) for activating CH 4 . Meanwhile, the ZCN Z -scheme heterostructure improves the migration and transport efficiency of photoexcitons but also enhances the activation and adsorption of CH 4. In situ experiments verify that the ZCN heterostructure accelerates the generation of methyl radical ( · CH 3 ) and · OH. This work paves a new way toward rationally constructing photocatalysts for CH 4 conversion into desirable chemical products under ambient conditions.
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OPTICAL MATERIALS
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2025
·
IF 4.2
Bo Li,Yujia Liu,Lishuai Song,Yuyu Zhang,Nan Liu,Zequan Li
Absrtact This study successfully constructs a g-C 3 N 4 /TiO 2 heterojunction and its Pt nanocluster-modified composite (Pt C –CN–TiO 2 ) through an interface engineering strategy, systematically investigating their photocatalytic RhB degradation performance and mechanisms. Under visible light irradiation, Pt C –CN–TiO 2 achieves a RhB degradation efficiency of 99.29 % within 160 min, with a 34.3 % increase in reaction rate constant compared to the Pt-free catalyst. Mechanistic studies reveal that Pt acts as an electron sink, facilitating the generation of ·O 2 − , while inducing interfacial electronic structure renormalization to enhance surface hydroxyl adsorption and oxygen vacancy activity. Cycling experiments confirm its exceptional stability. This work provides novel interface engineering insights and theoretical foundations for designing highly efficient and stable solar-driven photocatalysts.
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Catalysts
·
2025
·Vol. 15
·期 9
·808
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IF 4
Shuai Liu,Yipei Chen,Honglei Zhang,Yang Meng,Tao Wu,Guangsuo Yu
Constructing heterojunction photocatalysts with efficient interfacial charge transfer is critical for solar-driven hydrogen evolution. In this study, a highly dispersed MoS2/g-C3N4composite was successfully synthesized via a stirring-assisted hydrothermal in situ growth strategy. The introduction of stirring during synthesis significantly enhanced the uniform dispersion of MoS2nanosheets and exposed abundant edge sites, leading to well-integrated heterojunctions with enhanced interfacial contact. Comprehensive structural and photoelectronic characterizations (XRD, SEM, TEM, EDS mapping, UV–Vis, TRPL, EIS, EPR) confirmed that the composite exhibited improved visible-light absorption, accelerated charge separation, and suppressed recombination. Under simulated solar irradiation with triethanolamine (TEOA) as a sacrificial agent, the optimized 24% MoS2/g-C3N4-S catalyst achieved a high hydrogen evolution rate of 14.33 mmol·g−1·h−1at a catalyst loading of 3.2 mg, significantly outperforming the unstirred and pristine components, and demonstrating excellent cycling stability. Mechanistic studies revealed that the performance enhancement is attributed to the synergistic effects of Type-II heterojunction formation and edge-site-rich MoS2co-catalysis. This work provides a scalable approach for non-noble metal interface engineering and offers insight into the design of efficient and durable photocatalysts for solar hydrogen production.
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LANGMUIR
·
2025
·
IF 3.9
Xiao Zhang,Menglin Zhang,Zhiren Guo,Xiang Li,Ting Liu,Jinying Li,Dongxiang Zhang,Xiyan Xu
The persistent contamination of aquatic environments by tetracycline (TC) necessitates advanced remediation strategies. Herein, a ternary Fe–O–P-co-modified graphitic carbon nitride (FOPCNx) was synthesized via structural integration of Fe–N2 configurations with O/P dual doping for efficient TC degradation in a solar-driven photo-Fenton system. This study pioneers the synergistic coupling of Fe–N2 coordination and heteroatomic O/P substitution to optimize charge dynamics. Comprehensive characterization confirmed the formation of Fe–N2 active sites and aromatic structures incorporated with the aromatic group, which collectively enhanced visible-light absorption, suppressed electron–hole recombination, and facilitated charge carrier redistribution. The optimized FOPCN2 demonstrated exceptional photoelectric efficiency (3.7-fold higher photocurrent density than pristine g-C3N4) and achieved 98.9% TC removal within 40 min of irradiation with a kinetic constant of 0.113 min–1, outperforming conventional systems. Mechanistic studies revealed dual enhancement pathways: Fe–N2 sites promoted electron transfer and Fe(III)/Fe(II) cycling, while the O/P dual doping enabled electron delocalization for improved charge mobility. The system exhibited remarkable pH adaptability (3–7), robust resistance to inorganic anions, and universal degradation capability for mixed organic pollutants. Three TC degradation pathways were identified through intermediate analysis, with radical trapping and EPR verification confirming the dominant roles of •OH, e–, and O2•–. This work provides critical insights into structure–activity relationships for carbon nitride modification, establishing a paradigm for designing multifunctional photocatalysts for antibiotic-contaminated wastewater remediation.
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JOURNAL OF FLUORESCENCE
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2025
·
IF 3.1
Yao Jie,Chen Hongfang,Yang Xiaohua,Iqbal Muzaffar,Bian Wei
Mercury ions (Hg 2+ ) are categorized as environmental pollutants, which distributed in water, soil, and food systems due to environmental contamination. Hence, designing a sensitive assay for the convenient determination of Hg 2+ is of great importance. Herein, S and O-doped graphite phase nitrogenized carbon quantum dots (S, O-C 3 N 4 QDs) was encapsulated within a europium -based metal-organic framework (Eu-MOF) to construct a novel ratiometric fluorescent nanoprobe for the quantitative detection of Hg 2+ . The native emission of S, O-C 3 N 4 QDs at 445 nm is used as a response signal, while Eu-MOF with fluorescence offers a reference signal at 619 nm. Hg 2+ exhibits high affinity for the surface functional groups of S/O-C 3 N 4 QDs, forming non-fluorescent chelation complexes that induce static quenching. This results in significant attenuation of the fluorescence intensity at 445 nm, while the emission at 619 nm remains invariant. A ratiometric fluorescence sensing platform was established based on the intensity ratio (F 445 /F 619 ) for the selective detection of Hg 2+ . The linear range of S, O-C 3 N 4 QDs/Eu-MOF of Hg 2+ was 0.25–35 µM and with a detection limit of 4.3 nM. The satisfying results demonstrate the effectiveness of the developed S, O-C 3 N 4 QDs/Eu-MOF-based fluorescence probe for Hg 2+ detection, highlighting its promising potential for environmental monitoring applications.
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FUEL
·
2024
·
IF 6.7
Wenting Chen,Xinwei Zhao,Qi Zeng,Lili Liu,Pengju Yang,Shupeng Guo,Juzhi Leng,Min Zhong,Wei Hong,Lin Zhang
Combining the advantages of multiple strategies including morphology control, atom doping, and defect construction, the photocatalytic hydrogen evolution reaction (HER) performance of graphitic carbon nitride (g-C 3 N 4 ) may be boosted significantly. Herein, holey ultra-thin g-C 3 N 4 nanosheets (CNS-x, x = H, O, N) modified with structural vacancies and sulfur (S) dopant are synthesized through a straightforward method involving the pyrolysis of thiocyanuric acid under various gas atmospheres. The textural properties, type and concentration of structural defect, and S doping level are significantly influenced by the gas atmosphere. Remarkably, CNS-H with C, N dual defects and S-dopant exhibits the HER rate of 46.59 mmol·g −1 ·h −1 , which is 16.68 times higher than that of bulk g-C 3 N 4 . The corresponding apparent quantum yields are 17.24 % at 420 nm and 1.90 % at 520 nm. The enhanced HER performance of CNS-H can be attributed to the combined effect of improved charge separation, extended photoabsorption, and optimized properties of the platinum cocatalyst.
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ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
·
2024
·Vol. 31
·期 1
·1-13
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IF 3
Wu Jinze,Yao Jiale,Zhu Xiping,Zuo Danying,Zhang Hongwei,Jiang Shuai,Li Hongjun
Most hydrogels for dye treatment only have the adsorption ability for anionic or cationic dyes, while a few zwitterionic hydrogels that can adsorb both anionic and cationic dyes need a complicated regeneration process when they are reused. To prepare reusable zwitterionic adsorbent hydrogels, in this paper, a zwitterionic composite hydrogel with Ag@g-C 3 N 4 was prepared, which not only can adsorb both anionic and cationic dyes but also has photocatalytic degradation ability. The scanning electron microscopy images show that the optimum hydrogel has a large number of micro pores for dye adsorption. The adsorption capacity of the hydrogel achieves the highest in mixed dye concentration of 50 mg·L -1 with pH value of 7–9. Benefiting from the synergistic effect of adsorption and photocatalytic degradation, the removal efficiency of methyl orange and methylene blue in mixed dyes was up to 93.86% and 91.80%, respectively. The photocatalytic activity trapping experiments showed that superoxide radicals as well as hydroxyl radicals played a major role in photocatalytic degradation. After 5 consecutive photocatalytic degradations, the removal ratio of the hydrogel for dyes was still above 80%, indicating good photocatalytic degradation and reusability properties. This research suggested the zwitterionic composite hydrogel has a promising prospect in removing dyes from wastewater treatment.
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