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Polymers · 2023 ·Vol. 15 ·期 7 ·1781 · IF 5

Covalent Triazine Frameworks Decorated with Pyridine-Type Carbonitride Moieties: Enhanced Photocatalytic Hydrogen Evolution by Improved Charge Separation

Xianxian Kong,Fan Yang,Xiaoying Li,Mengying Fu,Tao Zeng,Shuang Song,Zhiqiao He,Yan Yu

A simple procedure of calcination under an Ar atmosphere has been successfully applied to create a covalent triazine framework bearing pyridine-type carbonitride moieties (PCN@CTF). The appending of PCN on the CTF led to visible light absorption at up to 600 nm in the UV/Vis diffuse-reflectance spectra. Photoluminescence and electrochemical impedance spectroscopy have been applied to clarify how modification of the CTF with PCN enhanced the separation efficiency of photoexcited charge carriers. An optimized 1%PCN@CTF sample showed the highest photocatalytic hydrogen evolution reaction (HER) rate of 170.2 ± 2.3 μmol g−1·h−1, 3.9 times faster than that over the pristine CTF. The apparent quantum efficiency of the HER peaked at (7.57 ± 0.10)% at 490 nm. This representative 1% PCN@CTF sample maintained continuous function for at least 15 h. This work provides new guidance for modification with PCN materials as a means of obtaining high photocatalytic efficiency and sheds light on the effect of appended pyridine rings on a CTF.Keywords:pyridine-type carbonitrides;covalent triazine frameworks;photocatalytic hydrogen evolution reaction;separation efficiency

研究领域: 材料科学 · 光催化
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ACTA PHYSICO-CHIMICA SINICA · 2024 · IF 10.8

Bimetallic AuCu Alloy Decorated Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Production

Wenxiu Yang,Jinfeng Zhang,Quanlong Xu,Yun Yang,Lijie Zhang

Covalent organic frameworks (COFs) represent a kind of novel crystalline porous organic substances with extended π -conjugation framework and tunable structures, which display great promise in photocatalysis. However, unadorned COFs suffer from sluggish reaction kinetics, and a cocatalyst is essentially needed to reduce the activation barrier toward specific surface reaction and accelerate reaction kinetics. In this work, bimetallic alloys serving as co-catalysts were decorated on COFs to enhance the photocatalytic hydrogen evolution performance. By precisely-tuning the ratio of AuCu alloy, the resultant Au 1 Cu 5 /COF-TpPa displays the highest photocatalytic hydrogen generation rate (8.24 mmol∙g −1 ∙h −1 ), even surpassing the Pt modified COF-TpPa (6.51 mmol∙h −1 ∙g −1 ). According to the systematic characterizations and theoretical calculation, Au 1 Cu 5 /COF-TpPa exhibits the significantly enhanced charge carrier separation efficiency and reduced H* formation energy barrier, thus possessing high photocatalytic performance. This work affords a valuable approach to advancing COF-based photocatalysts by employing bimetallic alloy cocatalysts. Download: Download high-res image (117KB) Download: Download full-size image

研究领域: 材料科学 · 光催化
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Catalysis Science & Technology · 2025 · IF 4.2

Construction of a 0D/2D NixP/LaTiO2N Schottky junction photocatalyst for efficient visible-light-driven photocatalytic CO2 reduction

Guoyu Xu,Yanan Chen,Peiling Lin,Zizhong Zhang,Tao Ji,Wenyue Su

Employing photocatalytic technology to transform CO2 into valuable fuels is considered a promising solution for addressing the exacerbated greenhouse effect and energy crisis. The development of photocatalysts featuring superior charge separation efficiency is pivotal for the widespread implementation of photocatalytic CO2 reduction technologies. Herein, zero-dimensional (0D) NixP nanoparticles are anchored onto two-dimensional (2D) LaTiO2N nanosheets by a photo-deposition method, and a NixP/LaTiO2N Schottky junction composite with excellent photocatalytic CO2 reduction performance is constructed. The optimal NixP/LaTiO2N composite achieves CO and CH4 yields of 9.39 and 4.15 μmol g−1 h−1, respectively, with the utilized photoelectron number (UPN) reaching 51.98 μmol g−1, which is approximately 9.7 times higher than that of LaTiO2N alone. The improved photocatalytic performance of the composites can be attributed to the formation of Schottky junctions, which effectively suppress the recombination of photogenerated carriers. This study provides a new idea for the development of 0D/2D Schottky junction photocatalysts.

CAS / MDL: 10277-43-7
研究领域: 材料科学 · 环境科学 · 能源科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Template Synthesis of Ag2S-Zn0.5Cd0.5S with two structures and their application in RhB’s Photodegradations

Yanyan Chen,Minghui Yu,Xiaoyu Gong,Yingjie Wang,Shenjie Li,Qi Hu,Shuang Wang,Hao Yu,Zhiqiang Li

Two kinds of Ag 2 S-Zn 0.5 Cd 0.5 S heterostructural photocatalysts were synthesized via a simple two-step hydrothermal method. The photochemical (PEC) properties of Zn 0.5 Cd 0.5 S nanoparticles modified by Ag 2 S are closely related to the reaction time of Zn 0.5 Cd 0.5 S nanoparticles. Compared with the Ag 2 S-Zn 0.5 Cd 0.5 S heterostructure prepared at low temperature, the Ag 2 S-Ag-Zn-Cd-S composite prepared at high temperature has higher charge transfer/separation efficiency and longer carrier life. The photocatalytic performance of Ag 2 S-Ag-Zn-Cd-S composites for the degradation of Rhodamine B (RhB) under visible light irradiation (λ = 420 nm) was significantly improved. The AZCS-180-4 h photocatalyst exhibited the highest degradation efficiency (83.1% within 40 min) with a rate constant of 0.0401 min −1 which exhibited prominent stability and repeatability, and can still maintain high photocatalytic activity after at least four cycles. Meanwhile, the study of photocatalytic mechanism shows that the photo-induced h + radical is the predominant active species in this photocatalytic system, followed by·OH and·O 2- play a secondary role.

研究领域: 材料科学 · 环境科学 · 化学
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Journal of Nanostructure in Chemistry · 2022 ·Vol. 13 ·期 5 ·481-495 · IF 8

Controllable construction of a three-dimensional spherical LaFeO3/Bi2O3 heterojunction with enhanced photocatalytic ability for tetracycline degradation

Jia Zi-ang,Zeng Qing-rui,Sun Yuan-bo,Feng Wei

A novel three-dimensional spherical LaFaO 3 /Bi 2 O 3 heterojunction was successfully constructed through a two-step synthesis, which included a biological template method and hydrothermal synthesis. Because of the addition of different quantities of LaFaO 3 , the as-prepared LaFaO 3 /Bi 2 O 3 composite showed different morphological structures, excitation energies, charge separation efficiencies, and degrees of photocatalytic performance. With the change in the amount of LaFaO 3 added, the morphology of the LaFaO 3 /Bi 2 O 3 complex changed from irregular clusters to a regular spherical structure. When the molar doping ratio of LaFaO 3 /Bi 2 O 3 was 1:2, it exhibited a near-perfect 3D spherical structure with external pyknotic grooves. The results of electrochemical impedance spectroscopy indicated that the 1:2 LaFeO 3 /Bi 2 O 3 catalyst exhibited the optimal charge separation efficiency. The bandgap of the prepared LaFaO3/Bi 2 O 3 composite changed from 1.95 eV (1:2) to 2.32 eV (3:4), which were lower than that of the Bi 2 O 3 template (2.81 eV). The 3D-spherical LaFaO 3 /Bi 2 O 3 catalyst almost completely removed 50 mg L −1 of tetracycline within 90 min. Electron spin resonance and radical trapping experiments revealed that radicals were the main oxidants in the photocatalytic reaction. The construction of a 3D floral spherically structured semiconductor composite photocatalyst improved the further degradation of tetracycline. Graphical abstract

研究领域: 材料科学 · 环境科学 · 化学工程
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Small · 2022 ·Vol. 18 ·期 21 ·2201332 · IF 15.153

Novel Cerium-Based Sulfide Nano-Photocatalyst for Highly Efficient CO2 Reduction

Hao Zhang,Jiamin Ma,Siyuan Wang,Jixiang Ji,Zhichao Zeng,Zhurui Shen,Yaping Du,Chun-Hua Yan

To address the environmental crisis caused by excessive emissions of CO 2 , the development of effective photocatalysts for the conversion of CO 2 into chemicals has emerged as one of the most promising strategies. Herein, beyond those well-studied materials, a rare-earth sulfide-based nanocrystal NaCeS 2 is fabricated and investigated for efficient and selective conversion of CO 2 into CO, where the role of Ce ions is crucial. Firstly, the hybridization of Ce 4f and Ce 5d orbitals contributes to the photoresponsive band structure of NaCeS 2 . Secondly, due to the charge rearrangement supplied by the incompletely filled 4f orbitals of Ce ions, NaCeS 2 exhibits excellent charge separation efficiency and CO 2 adsorption affinity, reducing the energy barrier for the conversion from CO 2 to CO. Moreover, a NaCeS 2 -MoS 2 heterostructure is also designed to further boost the electron transfer from the Mo site to the Ce site, which results in an improvement of the catalytic reduction yield from 7.24 to 23.42 µmol g −1 within 9 h (both better than TiO 2 controls). This work offers a platform for the development of rare-earth-based photocatalysts for CO 2 conversion.

CAS / MDL: 13463-67-7
研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Dual-pathway charge transfer mechanism of anatase/rutile TiO2-Ag3PO4 hollow photocatalyst promotes efficient degradation of pesticides

Junjie Ma,Yingguan Xiao,Juanrong Chen,Yue Shen,Sisi Xiao,Shunsheng Cao

Exploring high-performance photocatalysts still remains a big challenge due to poor charge separation efficiency. Herein, we prepare a novel anatase/rutile TiO 2 -Ag 3 PO 4 hollow photocatalyst (A/R-TiO 2 -Ag 3 PO 4 ) for addressing this challenge. Microstructural characterization and photoelectric measurements confirm that the synergy of hollow structure and dual-heterojunction can provide abundant active sites and boost efficient charge separation through dual-pathway charge transfer mechanism. The A/R-TiO 2 -Ag 3 PO 4 photocatalyst exhibits the highest photocurrent density (15.25 µA cm −2 ), which is 8.4 and 5.2 times than that of A-TiO 2 -Ag 3 PO 4 (1.82 µA cm −2 ) and P25-Ag 3 PO 4 (2.93 µA cm −2 ), respectively. Photo-degradation experiment shows that A/R-TiO 2 -Ag 3 PO 4 presents a high degradation percentage (98.7 %) of thiamethoxam (THX) within 30 min, which is 1.45 and 1.23 times than that of A-TiO 2 -Ag 3 PO 4 (68.1 %) and P25-Ag 3 PO 4 (80.7 %), respectively. Furthermore, the degradation percentage of THX by A/R-TiO 2 -Ag 3 PO 4 is as high as 96.4 % after seven successive cycles, indicating excellent cycling stability. Therefore, this work provides a new insight into exploring other high-performance photocatalysts by combining hollow structure and dual-heterojunction.

研究领域: 材料科学 · 环境科学 · 化学工程
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Journal of Semiconductors · 2016 ·Vol. 37 ·期 8 ·083004 · IF 0

Solvothermal synthesis of Bi2O3/BiVO4 heterojunction with enhanced visible-light photocatalytic performances*

Ying Wu,Jing Wang,Yunfang Huang,Yuelin Wei,Zhixian Sun,Xuanqing Zheng,Chengkun Zhang,Ningling Zhou,Leqing Fan,Jihuai Wu

Novel, three-dimensional, flower-like Bi2O3/BiVO4 heterojunction photocatalysts have been prepared by the combination of homogeneous precipitation and two-step solvothermal method followed by thermal solution of NaOH etching process. The as-obtained samples were fully characterized by X-ray diffraction, scanning electron microscopy, energy dispersive X-ray analysis, Brunauer-Emmett-Teller surface area, and UV—vis diffuse-reflectance spectroscopy in detail. The crystallinity, microstructure, specific surface area, optical property and photocatalytic activity of samples greatly changed depending on solvothermal reaction time. The photocatalytic activities of samples were evaluated on the degradation of methyl orange (MO) under visible-light irradiation. The Bi2O3/BiVO4 exhibited much higher photocatalytic activities than pure BiVO4 and conventional TiO2 (P25). The result revealed that the three-dimensional heterojunction played a critical role in the separation of the electron and hole pairs and enhancement of the interfacial charge transfer efficiency, which was responsible for the enhanced photocatalytic activity.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Designing S-scheme Au/g-C3N4/BiO1.2I0.6 plasmonic heterojunction for efficient visible-light photocatalysis

Benlin Dai,Xin Chen,Xiaofan Yang,Gang Yang,Shijie Li,Lili Zhang,Feihu Mu,Wei Zhao,Dennis Y.C. Leung

A novel S-scheme Au/g-C 3 N 4 /BiO 1.2 I 0.6 plasmonic heterojunction was constructed by calcining a mixture of flower-like BiOI and Au/g-C 3 N 4 nanosheets for the first time. This Au/g-C 3 N 4 /BiO 1.2 I 0.6 heterojunction exhibited excellent photocatalytic activity in bisphenol AF (BPAF) degradation and Cr(VI) reduction with high cycle stability under visible light irradiation. In particular, the photocatalytic performance of the optimum material developed (4-Au/g-C 3 N 4 /BiO 1.2 I 0.6 ) can reach 0.0174 min −1 (apparent rate of BPAF degradation) and 0.0204 min −1 (apparent rate of Cr(VI) reduction), which were 6.5 and 3.7 times that of pristine g-C 3 N 4 , respectively. The high photocatalytic performance was due to the high efficiency of charge separation, the excellent light absorption of localized surface plasmon resonance (LSPR) caused by the Au deposition, and the formation of S-scheme heterojunctions, which maintained strong photocatalytic reduction and oxidation activity. Noticeably, the charge density difference and band offsets of the g-C 3 N 4 /BiO 1.2 I 0.6 were calculated. The results revealed that an internal electric field (IEF) was created, which further demonstrated the formation of an S-scheme photocatalytic mechanism.

研究领域: 材料科学 · 环境科学
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2018 ·Vol. 18 ·期 7 ·4675-4683 · IF 1.354

Synthesis of Fe3O4/C with Cauliflower-Like BiVO4 for Improved Separation Efficiency of Charge Carriers and Photocatalytic Activity

Zhao Xiaoxu,Yi Chengwu,Zhang Menghan,Ma Changchang,Li Chunmei,Yan Yongsheng

Fe3O4/C/BiVO4 composite photocatalyst was fabricated successfully by a simple approach using yeast as a carbon source. Fe3O4/C/BiVO4 sample exhibited higher efficiency for photocatalytic degradation of tetracycline (TC) as compared to pure BiVO4 under visible light. In addition, after five recycles of photodegradation of TC, Fe3O4/C/BiVO4 showed a slight loss in photocatalytic activity, which confirmed its stability and long-time reusability. The photocatalytic mechanism was studied by active species trapping experiments, which revealed that the holes (h +) and superoxide radical (˙O− 2) played a key role in TC degradation. Moreover, photocatalyst could be easily recycled by an external magnetic field and reused without any loss in photocatalytic activity. This work provides a simple, eco-friendly and exemplary strategy for improving photodegradation activity of BiVO4-based photocatalyst.

研究领域: 材料科学 · 环境科学
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

α-Fe2O3/Cu2O(SO4) composite as a novel and efficient heterogeneous catalyst for photo-Fenton removal of Orange II

Xiaojun Guo,Yanan Xu,Fei Zha,Xiaohua Tang,Haifeng Tian

Hematite (α-Fe 2 O 3 ), as one of Fenton reagents, is widely investigated for the treatment of wastewater in the field of advanced oxidation processes (AOPs). Considering the fast charge carrier recombination of hematite (α-Fe 2 O 3 ), we have successfully synthesized a novel and high active heterogeneous Fenton catalyst α-Fe 2 O 3 /Cu 2 O(SO 4 ) for the degradation of organic pollutants. The results show that the as-obtained Cu 2 O(SO 4 )-Fe9 composite exhibits excellent degradation properties of Orange II. 98.9% degradation rate was achieved for 100 mL of 50 mg/L Orange II solution in the condition of 0.3 g/L Cu 2 O(SO 4 )-Fe9 catalyst, 3 mM H 2 O 2 and pH = 3.5. The degradation rate constants of Cu 2 O(SO 4 )-Fe9 in the photo-Fenton-like system are 9.33 and 4.07 times of Cu 2 O(SO 4 ) and α-Fe 2 O 3 , respectively. In addition, the mechanism and pathway for the degradation of Orange II were proposed. The scheme of combining copper-based oxysulfate Cu 2 O(SO 4 ) with hematite (α-Fe 2 O 3 ) could improve the efficiency of charge carrier separation, which will further enhance the catalytic activity and expand its application in water purification.

CAS / MDL: 7758-94-3
研究领域: 环境科学 · 催化化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Cd1-xNixS nanocrystals decorated flower-like Mn doped In2O3 microspheres with enhanced reduction activity of CO2

Yangfan Xu,Tianze Han,Tingting Ji,Wenqian Luan,Ruiyang Zhao,Jishu Han,Lei Wang

Photocatalytic CO 2 reduction technology provides a promising approach to solve the energy and environmental problems. In this work, flower-like MnIn 2 S 4 microspheres were prepared by solvothermal method , and then calcined in air to obtain flower-like Mn doped In 2 O 3 (Mn:In 2 O 3 ) microspheres . Subsequently, Ni doped CdS (Cd 1-x Ni x S) nanocrystals were prepared and compounded with Mn doped In 2 O 3 to obtain Cd 1-x Ni x S/Mn:In 2 O 3 composite photocatalysts . It was found that Cd 0 · 96 Ni 0 · 04  S/Mn:In 2 O 3 had the best photocatalytic CO 2 reduction activity. The CO yield reached to 43.40 μmol g −1 in 3 h. The improved CO 2 reduction property were attributed to not only the increased light absorption capacity and the expanded surface area but also the enhanced charge separation efficiency that caused by the construction of Z-scheme heterostructure . The design and preparation of high-efficiency photocatalyst would be an effective way to promote the development of photocatalytic CO 2 reduction.

研究领域: 材料科学 · 环境科学 · 能源科学
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