Journal of Materials Chemistry A
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2025
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IF 9.5
Han Liu,Jun Zhang,Quanlong Xu,Hong Tao,Tingmin Di,Quanrong Deng,Shenggao Wang
Artificial photosynthesis offers a viable strategy for sustainable and environmentally friendly H2O2 production. However, conventional inorganic semiconductor photocatalysts often face limitations such as restricted light absorption, inadequate redox ability, small specific surface area and poor stability, which greatly restrict their practical applications. Herein, an innovative inorganic/organic S-scheme heterojunction is fabricated by an electrostatic self-assembling method. The optimized BT-12 composite demonstrates a significantly enhanced photocatalytic H2O2 production rate of 723 μmol L−1, surpassing the rates achieved by pure Bi2WO6 and TpPa-Cl-COF by factors of 10 and 2.9, respectively. This improvement can be attributed to the synergistic effects of enhanced light absorption, increased specific surface area, and effective separation of charge carriers and redox active sites, as well as the strong redox ability induced by the S-scheme heterojunction. Density functional theory (DFT) calculations along with X-ray photoelectron spectroscopy (XPS) measurements and electron paramagnetic resonance (EPR) characterization confirm the step-by-step charge transfer pathway. The active species trapping experiments validate that H2O2 is predominantly produced by a two-step one-electron process. This work highlights an innovative and promising strategy for constructing a highly efficient photocatalytic system based on inorganic/organic heterojunctions.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Yuxuan He,Yongming Wang,Jin Qian,Kailin Xu,Bianhe Lu,Sijing Tang,Yin Liu,Junwei Shen
Photocatalysis for H 2 O 2 production suffers from low carrier utilization and slow reaction kinetics. Herein, a photocatalytic system supported by a SrCoO 3 -MoS 2 (SCOS) heterojunction, which possessed a unique S-O electron transport channel, was proposed to facilitate H 2 O 2 production under condition where glycerol served as a sacrificial agent. The SCOS heterojunction achieved a remarkable yield of 15.90 mmol g −1 h −1 H 2 O 2 production, 3.7 times higher than the base component SCO. The construction of the heterojunction enriched the oxygen vacancies on the catalyst surface, facilitated photogenerated charge separation, and promoted the adsorption of O 2 , reducing the oxygen reduction reaction (ORR) energy barrier. Besides, glycerol served as a unique proton donor, efficiently captured holes to enhance H 2 O 2 production, and generated valuable by-products including glyceric acid and dihydroxyacetone. Furthermore, SCOS exhibited excellent stability over repeated cycles with consistent H 2 O 2 yields. This study offers an efficient photocatalytic system and demonstrates glycerol’s potential in green oxidation processes.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
You Wu,Yi Yang,Miaoli Gu,Chuanbiao Bie,Haiyan Tan,Bei Cheng,Jingsan Xu
Solar photocatalysis is a promising, green, and sustainable technique for the synthesis of H 2 O 2 . In this study, low-dimensional ZnO/ZnIn 2 S 4 S-scheme heterojunction photocatalysts are fabricated using electrostatic spinning and chemical bath deposition methods for the efficient photocatalytic production of H 2 O 2 . ZnO nanofibers loaded with 20 wt% ZnIn 2 S 4 exhibit a superior H 2 O 2 production rate of 928 μmol g −1 h −1 , which is more than four times higher than that seen in pristine hexagonal phase ZnO and ZnIn 2 S 4 . First-principles calculations and in-situ X-ray photoelectron spectroscopy reveal the charge separation and transfer mechanisms in the S-scheme heterojunction. The construction of the S-scheme heterojunction facilitates the spatial separation of charge carriers, and electrons and holes with higher redox abilities are retained. Photoelectrochemical and photoluminescence tests further show that the formation of an S-scheme heterojunction is beneficial for the separation of photoinduced charge carriers. Electrochemical tests and electron paramagnetic resonance measurements indicate that H 2 O 2 production is primarily via a two-step single-electron O 2 reduction path. This study provides a new approach for the construction of S-scheme heterojunction materials that can efficiently produce H 2 O 2 under solar irradiation.
研究领域:
材料科学
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环境科学
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光催化技术
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 46
·22419-22426
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IF 3.925
Liran Liu,Hanping Fu,Yating Zeng,Li Feng,Tianxiang Zhang,Qingshuang Liang,Xiufeng Xiao
The development of high-efficiency economic photocatalysts for the production of hydrogen peroxide (H2O2) is of great significance for solar-to-fuel conversion. Bismuth oxychloride (BiOCl) shows great potential for photocatalytic H2O2 production, but the rapid recombination of electron–hole pairs reduces its photocatalytic performance. Herein, a series of Bi nanoparticle modified BiOCl (Bi/BiOCl) composites is constructed by an in situ chemical reduction to boost the spatial charge separation and transportation to enhance the photocatalytic performance for H2O2 production. Benefiting from the synergistic effects of localized surface plasmon resonance, the formation of Schottky barriers, and the in situ fabricated heterojunction that results in strong interfacial forces and tight contact, the obtained Bi/BiOCl composites exhibit enhanced photocatalytic capability for H2O2 production; the best sample can enable an impressive H2O2 production rate of 108 mmol g−1 h−1, which is much higher than that of individual BiOCl. The present work provides a clear understanding of the mechanisms of Bi nanoparticle modified BiOCl composites for photocatalytic H2O2 production, which will be useful for the development of catalysts toward solar-to-fuel conversion.
研究领域:
材料科学
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能源化学
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环境科学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Rong Ji,Yuming Dong,Xinyu Sun,Chengsi Pan,Yunfan Yang,Hui Zhao,Yongfa Zhu
Nowadays, considerable attention has been directed towards the two-electron oxygen reduction for the photocatalytic H 2 O 2 production. However, the challenge of insufficient charge separation capacity markedly constrains the rate of H 2 O 2 production. Herein, we designed a donor-acceptor (D-A) interface characterized by rapid charge migration and separation to enhance the photocatalytic H 2 O 2 production. Specifically, naphthalenetetracarboxylic acid-diaminotriazole as an organic molecule has been judiciously chosen as the electron donor, while perylenetetracarboxylic acid serves as the electron acceptor. The novel semiconductor with D-A interface performs markedly strong internal electric field and demonstrates an excellent H 2 O 2 production rate of 3176 μM h −1 . The pronounced internal electric field facilitated by the D-A interface effectively expedites charge separation and induces the migration of photogenerated carriers to the O 2 reduction sites. This study introduces a novel paradigm for the design of D-A interfacial organic materials aimed at realizing enhanced photocatalytic capabilities.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Entong Ye,Fangmei Lin,Chengbin Fu,Xin Zhou,Qian Lin,Hongyan Pan,Zheng Chen
A great deal of research has been carried out on the design of Pd-based catalysts in the direct synthesis of H2O2, mainly for the purpose of improving the H2O2 selectivity by weakening the activation energy on the Pd active site and thus inhibiting the dissociation of the O–O bonds in O2*, OOH*, and HOOH*. However, this often results in insufficient activation energy for the reaction between H2 and O2 on Pd, leading to difficulties in improving both the selectivity and productivity of H2O2 simultaneously. Based on this, this study reports an efficient catalyst composed of amine-functionalized SBA-15-supported Pd. The strong metal–support interaction not only makes the PdNPs highly dispersed with more Pd active sites but also improves the stability of the catalyst. The amine group modification increases the proportion of Pd0, further enhancing Pd activity and promoting the adsorption and conversion of H2 and O2 on Pd, thereby significantly increasing H2O2 productivity. Additionally, the density-functional theory simulation results showed that due to the hydrogen-bonding force between the amine group and H2O2, this particular anchoring effect would make the hydrogenation and decomposition of H2O2 effectively suppressed. Ultimately, both the selectivity and productivity of H2O2 are improved simultaneously.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
Yiming Chen,Wenquan Gu,Li Tan,Zhimin Ao,Taicheng An,Shaobin Wang
Photocatalytic H 2 O 2 production by O 2 reduction is an environmental-friendly process for solar light conversion to chemical energy. In this work, Ti 3 C 2 MXene was used as a non-noble metal cocatalyst to load on P25 as Ti 3 C 2 /TiO 2 (TC/TO) photocatalysts for photocatalytic H 2 O 2 synthesis. A H 2 O 2 formation rate (179.7 μmol L −1 h −1 ) of the optimized 10 %-TC/TO composite was obtained to be over 21 folds as high as that of P25 under UV light. Radical quenching experiments and superoxide radical detection confirmed the superoxide radical as the primary intermediate, suggesting the O 2 reduction in two-step single-electron indirect reaction. The higher activity of TC/TO can be attributed to the functions of Ti 3 C 2 MXene in accelerating the separation and transfer of photogenerated electron-hole pairs, suppressing their recombination, and blocking the surface Ti OOH formation. This work proves the promising roles of Ti 3 C 2 MXene in the photocatalytic reaction and further expands their new applications in photocatalysis .
研究领域:
材料科学
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环境化学
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光化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Han Zhang,Xuefeng Bai
Photocatalytic H 2 O 2 production is an eco-friendly technique because only H 2 O, molecular O 2 and light are involved. However, it still confronts the challenges of the unsatisfactory productivity of H 2 O 2 and the dependence on organic electron donors or high purity O 2 , which restrict the practical application. Herein, we construct a type-II heterojunction of the protonated g-C 3 N 4 coated Co 9 S 8 semiconductor for photocatalytic H 2 O 2 production. The ultrathin g-C 3 N 4 uniformly spreads on the surface of the dispersed Co 9 S 8 nanosheets by a two-step method of protonation and dip-coating, and exhibits improved photogenerated electrons transportability and e - -h + pairs separation ability. The photocatalytic system can achieve a considerable productivity of H 2 O 2 to 2.17 mM for 5 h in alkaline medium in the absence of the organic electron donors and pure O 2 . The optimal photocatalyst also obtains the highest apparent quantum yield (AQY) of 18.10% under 450 nm of light irradiation, as well as a good reusability. The contribution of the type-II heterojunction is that the migrations of electrons and holes within the interface between g-C 3 N 4 and Co 9 S 8 matrix promote the separation of photocarriers, and another channel is also opened for H 2 O 2 generation. The accumulated electrons in conduction band (CB) of Co 9 S 8 contribute to the major channel of two-electron reduction of O 2 for H 2 O 2 production. Meanwhile, the electrons in CB of g-C 3 N 4 participate in the single electron reduction of O 2 as an auxiliary channel to enhance the H 2 O 2 production.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Yu Wang,Yuxin He,Yujing Chi,Peiji Yin,Lishan Wei,Wenwen Liu,Xinyao Wang,Han Zhang,Haiyan Song
Photocatalytic H 2 O 2 production is a green and sustainable technology, which still exposes the issues of excessive dependence on organic electron donors and pure O 2 , and lacking effective use. It is necessary to develop more efficient and more economical photocatalysis system for H 2 O 2 production. Here, we construct a S-scheme p-n heterojunction from the p-type MnS and the n-type protonated g-C 3 N 4 (PCN) semiconductors for photocatalytic H 2 O 2 production and achieve the in situ use of H 2 O 2 for oxidative degradation of oxytetracycline (OTC). The PCN/MnS composite synthesized by a one-step method well maintains a nanosphere structure of α-MnS and load the PCN on the sphere surface to form a heterojunction with strong interaction. PCN/MnS exhibits the improved photogenerated charge separation and electron transfer efficiency. An optimal photocatalyst can produce 669.6 μM of H 2 O 2 for 6 h without using the electron donors and the pure O 2 gas. The mechanism proposed the contribution of a S-scheme p-n heterojunction forms between PCN and MnS. The electrons in conduction band (CB) of MnS are responsible for the major single-electron reduction of •O 2 - radicals and the auxiliary two-electron reduction of O 2 for H 2 O 2 production, while the holes in valence band (VB) of PCN further promote the separation of photocarriers. The photogenerated H 2 O 2 can be effectively used as an in-situ oxidant to achieve 82.2% degradation of OTC in water within 80 min. The •O 2 - radicals which originate from the in situ decomposition of H 2 O 2 over PCN/MnS mainly contribute to the OTC oxidation .
研究领域:
材料科学
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环境科学
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光化学
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催化
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Dengyu Fu,Yanji Zhu,Lei Chen,Yue Sun,Meng Zhang,Huaiyuan Wang
Heteroatom modified catalyst applying for the two-electron oxygen reduction reaction has the potential application for efficient on-site production of H 2 O 2 . At present, state of the art catalyst synthesis is often energy-intensive and tends to destroy the original structure of heteroatoms. Based on the above considerations, Co-O, pyrrolic N structures co-modified graphite felt catalyst (Co-PDA-GF) is successfully synthesized by a simple two-step electrochemical method . Interestingly, the introduction of Co 2+ during the dopamine (DA) polymerization process changes the surface morphology of GF from a “thin-film” like to an “ant-nest” like. The cumulative H 2 O 2 concentration achieves 421 mg L −1 in 6 h test time, which is 16 times higher than that of R-GF, and the Methylene blue (MB) in-situ removal rate reaches 97.2% within 3 h. The enhanced H 2 O 2 yield of Co-PDA-GF catalyst is attributed to the increased oxygen-containing functional groups (-COOH, -C-O-C) and defect structures , and most importantly, Co-O and pyrrolic N synergistic modulation effects on local electronic modulation. This work provides new insights on DA polymerization morphology control and designing of high-efficient 2e − ORR catalyst with a low-energy method.
研究领域:
电化学
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材料科学
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催化
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环境化学
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高影响因子
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