MOLECULES
·
2026
·Vol. 31
·期 4
·740
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IF 5.1
Quan Xiang,Linzhu Zhang,Lu Chen,Ruowen Liang,Renkun Huang,Guiyang Yan
Catalytic systems that couple pollutant degradation with hydrogen evolution have attracted significant attention due to their potential to simultaneously address environmental and energy issues. In this study, an S-scheme heterojunction composed of lamellar polymeric carbon nitride (PCN) anchored with a rod-like cerium metal–organic framework (Ce-MOF) was successfully synthesized via a facile one-step oxidation method, enabling efficient visible-light-driven photocatalytic hydrogen evolution and simultaneous tetracycline degradation. The optimized PCN/Ce-MOF composite delivers a hydrogen production rate of 495.7 μmol g−1h−1and achieves a tetracycline removal efficiency of 78%. Such excellent performance is attributed to the charge transfer mechanism of the S-scheme heterojunction in the PCN-Ce-MOF composite during the reaction process, while retaining the intrinsic redox capabilities of both materials. Meanwhile, mechanistic studies reveal that tetracycline can effectively capture holes during its efficient degradation, inhibit electron–hole recombination, and promote proton reduction to generate hydrogen. This investigation provides valuable insights for the rational design of S-scheme heterojunction photocatalysts, aiming to achieve efficient and stable photocatalytic hydrogen production and synergistic degradation of organic pollutants.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Haodong Sun,Zuoyi Xiao,Zhenyu Zhao,Shangru Zhai,Qingda An
Accelerating the charge separation efficiency is a crucial approach to improve the photocatalytic performance of semiconductors. The design and synthesis of heterojunctions can effectively inhibit the recombination of photogenerated electron-hole pairs and enhance the charge separation efficiency. In this work, an easy-handling calcination route was proposed to prepare CdS/ZnS heterojunction loaded on honeycomb-like porous carbon (CZS@C) using chitosan as a precursor. The unique honeycomb-like porous structure facilitated the separation and migration of photoexcited electrons and holes, improving the utilization of visible light and shortening the distance of electron transport. The photocatalytic performance of CZS@C was evaluated by the degradation of tetracycline (TC) and H 2 production from water splitting under visible light. The optimized CZS@C composite can degrade almost 92.40 % of TC under visible light irradiation in 60 min. Such CZS@C composite presented an excellent photocatalytic activity with H 2 production rate of 5.49 mmol h −1 g −1 , which was 54.9 and 2.28-folds higher than ZnS@C and CdS@C. Furthermore, the possible photocatalytic reaction mechanism and pathway towards TC degradation and simultaneous H 2 generation was proposed.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Fang-Yuan Bai,Jing-Ru Han,Jun Chen,Yue Yuan,Ke Wei,Yuan-Sheng Shen,Yi-Fu Huang,Heng Zhao,Jing Liu,Zhi-Yi Hu,Yu Li,Bao-Lian Su
Glucose conversion assisted photocatalytic water splitting technology to simultaneously produce H 2 and high value-added chemicals is a promising method for alleviating the energy shortage and environmental crisis. In this work, we constructing type II heterojunction by in-situ coupling Zn 0.3 Cd 0.7 S quantum dots (ZCS QDs) on three-dimensionally ordered microporous CaTiO 3 (3DOM CTO) for photocatalytic H 2 production and glucose conversion. The DFT calculations demonstrate that substitution of Zn on the Cd site improves the separation and transmission of photogenerated carriers. Therefore, 3DOM CTO-ZCS composite exhibits best H 2 production performance (2.81 mmol g -1 h −1 ) and highest apparent quantum efficiency (AQY) (5.56 %) at 365 nm, which are about 47 and 18 times that of CTO nanoparticles (NPs). The improved catalytic performance ascribed to not only good mass diffusion and exchange, highly efficient light harvesting of 3DOM structure, but also the efficient charges separation of type Ⅱ heterojunction. The investigation on photocatalytic mechanism indicates that the glucose is mainly converted to gluconic acid and lactic acid, and the control reaction step is gluconic acid to lactic acid. The selectivity for gluconic acid on 3DOM CTO-ZCS is 85.65 %. Our work here proposes a green sustainable method to achieve highly efficient H 2 production and selective conversion of glucose to gluconic acid.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Fangshu Xing,Renyou Zeng,Chuchu Cheng,Qiuwen Liu,Caijin Huang
Efficient aromatic alcohol oxidation with simultaneous H 2 evolution under aqueous conditions is achieved in a polyoxometalate (POM)-incorporated ZnIn 2 S 4 dual-functional photocatalytic system. The synergy between HPM and ZIS contributes to the formation of a Z-type heterojunction structure and thus enhances redox capacity. Moreover, the sub-nanometer size of POM clusters endows molecular-level interfacial contact, which acts as an "electron bridge" ensuring faster interfacial charge transfer kinetics. Therefore, an impressive nearly 100% yield of benzaldehyde and 10.6 mmol·g −1 ·h −1 H 2 -evolution rate are observed for POM/ZIS nanocomposites even under an anaerobic atmosphere with water as the solvent. This is the first application of POM-based materials in the anaerobic oxidation of benzyl alcohol with concomitant H 2 production. This study expands the possibilities for designing multifunctional POM-based photocatalysts for economic and ecological photoredox applications.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Xiaohui Yu,Haiwei Su,Jianping Zou,Qinqin Liu,Lele Wang,Hua Tang
ABSTRACT Durable and inexpensive graphitic carbon nitride (g-C 3 N 4 ) demonstrates great potential for achieving efficient photocatalytic hydrogen evolution reduction (HER). To further improve its activity, g-C 3 N 4 was subjected to atomic-level structural engineering by doping with transition metals (M = Fe, Co, or Ni), which simultaneously induced the formation of metal–N active sites in the g-C 3 N 4 framework and modulated the bandgap of g-C 3 N 4 . Experiments and density functional theory calculations further verified that the as-formed metal–N bonds in M-doped g-C 3 N 4 acted as an “electron transfer bridge”, where the migration of photo-generated electrons along the bridge enhanced the efficiency of separation of the photogenerated charges, and the optimized bandgap of g-C 3 N 4 afforded stronger reduction ability and wider light absorption. As a result, doping with either Fe, Co, or Ni had a positive effect on the HER activity, where Co-doped g-C 3 N 4 exhibited the highest performance. The findings illustrate that this atomic-level structural engineering could efficiently improve the HER activity and inspire the design of powerful photocatalysts.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Jie-wen Liu,Jian Zhang,Ming-jie Xu,Chuan-jin Tian,Xiao-jun Zeng,Chang-an Wang
Developing highly active and reliable Pt-based catalysts is a major challenge for the widespread commercialization of proton-exchange membrane fuel cells. Herein, we have designed Pt3Co@C hollow sphere catalysts by the template method, in which PtCo alloy nanoparticles of approximately 3 nm diameter are anchored in a porous shell of nitrogen-doped carbon hollow spheres. Due to the confinement effect of the porous carbon shell, PtCo alloy nanoparticles possess excellent resistance to sintering, maintaining 2–3 nm size after calcination at 800 °C. Also, Pt3Co@C hollow sphere catalysts exhibit superior catalytic activity and stability in the oxygen reduction reaction, achieving 3.6 times the mass activity of the corresponding commercial Pt/C catalyst. Such catalysts with a mass activity retention rate of 87% after accelerated durability testing and no significant decay in activity after 10,000 potential cycles. Meanwhile, Pt3Co@C catalysts exhibit extremely high catalytic activity and surprising durability for the hydrogen evolution reaction process over the entire pH range. We believe that this methodology provides an insight into the preparation of high-performance electrocatalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Ya Xiong,Teng Liu,Xinyu Wang,Wendi Liu,Yanjun Xue,Xiaoli Zhang,Can Xiong,Jian Tian
Ultrathin CdS nanosheets (NSs) are intriguing in photocatalytic hydrogen evolution . Severe photo-corrosion and rapid recombination of electrons and holes, however, impair their applications. To solve this problem, a novel step-scheme (S-scheme) 2D CdS/W 18 O 49 heterostructure with strong interfacial interactions and large contact interface has been successfully designed. Due to the ultrathin structure of CdS, defect-rich W 18 O 49 NSs-assembled network, unique 2D heterostructure and state-of-the-art S-scheme mode, 40 wt% CdS/W 18 O 49 (CW40) shows a prominent photocatalytic H 2 production rate of 15.4 mmol g −1 h −1 . Besides, the apparent quantum efficiency of CW40 is up to 15.4 % under light at λ = 370 nm. Besides, the as-prepared CW40 can protect CdS from photo-corrosion, exhibiting outstanding stability over 24 h circular reaction. Our work provides an out-of-box solution to broaden the application potential of certain catalysts with inherent drawbacks and offers fresh insight into the design and preparation of highly-efficient 2D heterostructures for versatile applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yunfeng Qiu,Xiaofan Dai,Yanping Wang,Xinyang Ji,Zhuo Ma,Shaoqin Liu
It is urgent to develop non-noble metal electrocatalysts with both excellent activity and durable stability for H 2 production via water electrolysis. Electric energy is mainly consumed by the sluggish anodic oxygen evolution reaction (OER). The electrocatalytic urea oxidation reaction (UOR) has been regarded as a promising reaction to replace OER because of its small thermodynamic oxidation potential . However, developing a facile and large-scale preparation method for bifunctional hydrogen evolution reaction (HER) and UOR electrocatalysts is still challenging. Herein, phosphate-modified (4.46 atomic%) NiMoO 4−x net-like nanostructures are formed on Ni foam (NF) via H 3 PMo 12 O 40 etching strategy at room temperature (denoted as NF/P-NiMoO 4−x ). The etched NF can directly serve as HER electrode , and delivers overpotential of 116 mV at current density of 10 mA/cm 2 with Tafel slope of 77.5 mV/dec. Furthermore, it displays excellent UOR activity with potential of 1.359 V at current density of 10 mA/cm 2 and Tafel slope of 19.3 mV/dec. The apparent activation energy of NF/P-NiMoO 4−x is 20.6 kJ/mol, lower than that of NF (37.7 kJ/mol), indicating smaller apparent barrier for C N bond cleavage in urea. The cell voltage of urea electrolysis is around 1.48 V for H 2 production to deliver current density of 10 mA/cm 2 , and better long-term stability for 50 h than that of Ir/C||Pt/C. The etching solution can be recycled for five times by addition of H 2 O 2 , turning heteropoly blue into its original state. This work develops a facile and large-scale method to prepare bifunctional HER and UOR electrocatalysts for H 2 production in a less-energy saving way via urea electrolysis.
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CRYSTENGCOMM
·
2022
·Vol. 24
·期 28
·5141-5148
·
IF 3.756
Yan Ma,Dianjun Chi,Yuping Tao,Shengjun Liu,Lei Dong,Yu Chen,Lifang He,Kui Zhang
Catalysts with low cost, high efficiency, and no need for precious metal cocatalysts are the key to realizing the maximum utilization of solar energy-efficient hydrogen (H2) production. In this study, a series of graphitic carbon nitride-derived catalysts (g-C3N4/CoP@C) were successfully obtained by in situ phosphating of g-C3N4/Co-BDC. A CoP@C cocatalyst developed with Co-BDC nanosheets as precursors can accelerate the H2 generation of g-C3N4. The close interface between CoP@C and g-C3N4 increased the electron–hole separation efficiency. Moreover, the CoP@C surface carbon accelerated electron transfer and increased the light absorption range. The prepared g-C3N4/CoP@C composite material exhibited H2 production capability up to 1968 μmol g−1 (3 h), approximately 129.9 times that of g-C3N4. Therefore, the CoP@C cocatalyst is proposed as an alternative to non-precious metal cocatalysts based on the findings of the study.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ye Meng,Yumei Jian,Jie Li,Hongguo Wu,Heng Zhang,Shunmugavel Saravanamurugan,Song Yang,Hu Li
The appropriate regulation of photocatalyst band structure by simultaneous introduction of active sites is an effective strategy in constructing efficient photocatalytic systems for biomass valorization. Herein, a renewed host–guest photocatalyst (Ov-WO 3 @CB[5]) prepared by anchoring cucurbit[5]uril on oxygen vacancy-rich WO 3 was efficient for reductive upgrading of biomass derivatives using NH 3 -BH 3 , such as cascade photocatalytic hydrogenation-cyclization of ethyl levulinate to γ-valerolactone (up to 99 % yield) at 25 °C in 1 h, and quantitative production of primary/secondary bio-alcohols or arylamines from various aldehydes/ketones or nitroarenes, respectively. Also, the rate of H 2 production by direct photocatalytic hydrolysis of NH 3 -BH 3 could reach 5.75 mL h −1 g −1 . The inclusion of cucurbit[5]uril effectively adjusted the semiconductor band structure and enhanced migration efficiency of photo-generated carriers, and the hydrophobic cavity of cucurbit[5]uril favored the entrance of NH 3 -BH 3 , as elaborated by theoretical calculations. Properly engineering supramolecular surface-active sites based on interface host–guest chemistry opens new avenues for reductive upgrading of biomass and hydrogen evolution.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Chenhao Sun,Fangqin Li,Jianxing Ren,Jiang Wu,Guanjun Wang,Linfeng Chen
Exploring low-cost and earth-abundant photocatalysts to efficiently release H 2 from wastewater is an appealing solution for global energy and environmental issues. Here, we successfully prepared flower-like 1T/2H-MoS 2 -decorated g-C 3 N 4 (thiourea)/g-C 3 N 4 (urea) (denoted as CNT/CNU) isotype heterojunction photocatalysts via a facile ultrasonic dispersion method and researched the photocatalytic H 2 generation and pollutant degradation performance in oxalic acid (OA) simulated wastewater. The results displayed that 20% 1T/2H-MoS 2 @CNT/CNU sample exhibited the highest photoreactivity, and the H 2 release rate was 1563.32 μmolg -1 h −1 , which was about 96 times higher than the CNT/CNU. Meanwhile, it also showed the highest total organic carbon (TOC) removal rate of 67.5%. The increased photoreactivity of nanocomposites can be ascribed to the double-interface system to effectually improve the separation of photoinduced charges. Additionally, the experimental results further confirmed that the loading of flower-like 1T/2H-MoS 2 could provide abundant active sites as well as expand the visible-light absorption range. Significantly, photoelectrochemistry measurements and density functional theory (DFT) calculations also confirmed that 1T/2H-MoS 2 cocatalysts accelerated the charge migration. On this basis, the mechanism of 1T/2H-MoS 2 @CNT/CNU promoting hydrogen production and synergistic OA degradation was proposed. This research presents a prospective idea for the utilization of waste water and the simultaneous production of clean energy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lin Wei,Deqian Zeng,Jieqian Liu,Hongfei Zheng,Toyohisa Fujita,Minyi Liao,Chunyi Li,Yuezhou Wei
Metal selenide semiconductors have been rarely used for photocatalytic water splitting because of their poor stability and severe photocorrosion properties. Hence, designing stable metal selenides with suitable bandgap energies has considerable practical significance in photocatalytic H 2 evolution. In this work, a novel series of Zn x Cd 1-x Se (x = 0 ∼ 1) with tunable band structure were fabricated through a simple solvothermal method. Impressively, the ZnSe exhibited a maximum H 2 production rate of 1056 µmol g −1 h −1 , which was higher than that of CdSe and Zn x Cd 1-x Se solid solutions. Such visible-light photoactivity for water reduction to H 2 was attained even after 6 cycling photocatalytic experiments. Moreover, the two-dimensional (2D) Ni 2 P nanosheets act as a high-efficiency cocatalyst integrated with Zn x Cd 1-x Se semiconductor to boost photocatalytic H 2 generation performance. The optimal 8% Ni 2 P/ZnSe composites displayed excellent cycling stability and superior photocatalytic H 2 evolution performance (4336 µmol g −1 h −1 ), which was about 4.1 times that of pure ZnSe under visible light irradiation. Photoelectrochemical (PEC), photoluminescence (PL), and time-resolved photoluminescence (TRPL) measurements reveal that the improved photoactivity Ni 2 P/ZnSe photocatalysts were ascribed to the effective separation and migration of photoinduced carriers. The present work paves a pathway to explore the fabrication of Zn x Cd 1-x Se solid solutions and the hybridization of 2D transition metal phosphides nanosheets toward photocatalytic applications.
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