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Catalysts · 2018 ·Vol. 8 ·期 4 ·147 · IF 3.465

Enhancing Light-Driven Production of Hydrogen Peroxide by Anchoring Au onto C3N4 Catalysts

Xiaoyu Chang,Junjiao Yang,Dandan Han,Bing Zhang,Xu Xiang,Jing He

Light-driven production of hydrogen peroxide (H2O2) is a green and sustainable way to achieve solar-to-chemical energy conversion. During such a conversion, both the high activity and the stability of catalysts were critical. We prepared an Au-supported C3N4catalyst—i.e., Au/C3N4-500(N2)—by strongly anchoring Au nanoparticles (~5 nm) onto a C3N4matrix—which simultaneously enhanced the activity towards the photosynthesis of H2O2and the stability when it was reused. The yield of H2O2reached 1320 μmol L−1on Au/C3N4-500(N2) after 4 h of light irradiation in an acidic solution (pH 3), which was higher than that (1067 μmol L−1) of the control sample Au/C3N4-500(Air) and 2.3 times higher than that of the pristine C3N4. Particularly, the catalyst Au/C3N4-500(N2) retained a much higher stability. The yield of H2O2had a marginal decrease on the spent catalyst—i.e., 98% yield was kept. In comparison, only 70% yield was obtained from the spent control catalyst. The robust anchoring of Au onto C3N4improved their interaction, which remarkably decreased the Au leaching when it was used and avoided the aggregation and aging of Au particles. Minimal Au leaching was detected on the spent catalyst. The kinetic analyses indicated that the highest formation rate of H2O2was achieved on the Au/C3N4-500(N2) catalyst. The decomposition tests and kinetic behaviors of H2O2were also carried out. These findings suggested that the formation rate of H2O2could be a determining factor for efficient production of H2O2.Keywords:hydrogen peroxide;Au catalyst;photosynthesis;carbon nitride

CAS / MDL: 16961-25-4
研究领域: 化学 · 材料科学 · 环境科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 · IF 3.9

Improved H2O2 photogeneration on KBr doped-polymeric carbon nitride via optimize the oxygen reduction path

Ziyu Liu,Xinyu Wang,Pengye Zhang,Haonan Zhang,Shuai Wang,Gaiyan Jiao,Wenting Wu,Mingbo Wu

The photosynthesis of hydrogen peroxide (H2O2) from oxygen (O2) represents a promising catalytic pathway, the limited efficiency of the oxygen reduction constitutes a primary barrier to enhancing production. In this content, alkali metal potassium (K+) and Br-doped g-C3N4 photocatalysts (K-CN) were successfully constructed by one-pot method. The introduction of K+ is not only beneficial to the transmission of space charge and the separation efficiency of photogenerated carriers, but also promotes the efficient production of H2O2 by 2e- oxygen reduction reaction. The introduction of Br- promotes O2 converted to triplet state and triggers energy transfer process to increase 1O2 production, O2 adsorption was facilitated through regulating the oxygen evolution (O2→1O2), which is beneficial to the subsequent oxygen reduction process. The results showed that the H2O2 yield of 0.05 K-CN catalyst reached 26.0 mmol g-1 h-1, which was more than 5 times that of pure g-C3N4.

CAS / MDL: 62-56-6
研究领域: 材料科学 · 催化化学
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

One-Step Laser Synthesis of Dual-Atom Alloy Catalysts for Hydrogen Evolution Reaction

Ran Zhang,Jiyun Chen,Yihe Huang,Jianai Tang,Rongxia Zhao,Yuxiang Liu,Lei Lei,Degao Wang,Lin Li,Zhu Liu

Recently, dual-atom alloy (DAA, also named diatomic alloy) catalysts with active metal dimers supported by a less active host metal have attracted considerable interest owing to their distinctive geometric and electrical configurations. Despite developing many ways for synthesizing DAA catalysts, most contemporary methods depend on high-temperature pyrolysis, costly apparatus, and intricate procedures. This study presents, for the first time, a one-step laser solid-phase synthesis of (PtRu) 1 Co DAAs on low-defect graphene support via ultraviolet (UV) laser irradiation of mixed metal precursors on a ZIF-67@PBI composite support. The special structure enhances the catalytic performance for hydrogen evolution reaction (HER) in an alkaline solution. An overpotential of 27 mV is reached at a current density of -10 mA cm⁻ 2 . The mass activity at 200 mV is 19.6 times more than that of the commercial Pt/C catalyst. Moreover, the catalytic activity sustained stability over 100 h at -200 mA cm −2 . The results demonstrated the potential of laser solid-phase synthesis as a viable method for synthesizing DAA catalysts via precise controlling defect formations on metal nanoparticles and carbon support. This one-step laser technique is rapid and cost-effective and opens up a new avenue toward large-scale synthesis of DAA catalysts.

CAS / MDL: 693-98-1 7440-06-4
研究领域: 材料科学 · 化学工程 · 纳米技术
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Laser-assisted rapid synthesis of anatase/rutile TiO2 heterojunction with Function-specified micro-zones for the effective photo-oxidation of sulfamethoxazole

Shilan Zhang,Songsong Zhi,Hongju Wang,Jing Guo,Weihao Sun,Lu Zhang,Yi Jiang,Xiaguang Zhang,Kai Jiang,Dapeng Wu

A solid-state laser scanning treatment (SLST) was adopted to synthesize anatase/rutile TiO 2 heterojunction with effective charge carrier separation and high surface adsorption performances for the photodegradation of sulfamethoxazole (SMX). The 1064 nm pulsed fiber laser could in-situ generate rutile zones on the pristine sheet-like anatase crystal enclosed by (0   0   1) facets, which could form the well-defined anatase/rutile interface to promote the formation of dominating active species ( h + and ∙OH) on the anatase zones. X-ray absorption fine structure (XAFS) measurements, low temperature electron paramagnetic resonance (LT-EPR) as well as the density functional theory (DFT) simulation proved that the oxygen vacancies (V O ) could both introduce defective energy states to promote the light absorption and enhance the SMX adsorption on anatase zones. Based on the delicately designed micro-zones, the photodegradation efficiency of the optimized catalyst could reach 99.3 %, which demonstrated ∼7 times higher performance than that of pristine TiO 2 and exhibited robust stability under environmental conditions. Gaussian and Vienna Ab Initio Package (VASP) programs were used to provide detailed degradation pathways and mechanism for SMX. This SLST could be potentially employed to create function-specified zones on various catalysts for different applicational aims.

研究领域: 材料科学 · 环境科学 · 化学工程
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SYNTHETIC METALS · 2020 · IF 3.286

Self-feedback autocatalysis in free radical triggered photosynthesis of N-doped graphene quantum dots

Yucheng Yang,Siwei Yang,Guqiao Ding,Zhi Liu

Much attention has been focused on the fabrication approaches of graphene quantum dots (GQDs) with efficient, time-saving, environmentally friendly and controllable approaches, which is well relevant to further applications. In this paper, we demonstrated the self-feedback autocatalysis progress in photosynthesis of N doped GQDs (N-GQDs). N-GQDs can be obtained via the simple ultraviolet (UV) irradiation for the mixture of urea, citric acid (CA) and H 2 O 2 . No by-product was generated during the preparation process and the yield of N-GQDs is 94 wt%. Compared with GQDs obtained via previously reported methods, the highly homogeneous size of these N-GQDs (2.4–3.1 nm) demonstrated the outstanding morphological control capacity of our suggested approach. More importantly, we demonstrated the self-feedback autocatalysis progress is the key factor for the suggested efficient preparation approach. Such self-feedback autocatalysis polymerization progress under ultraviolet irradiation is a rapid and effective method to obtain N-GQDs with good morphology and optical properties . This ultraviolet excitation-induced mechanism can be a universal method for numbers of nitrogen-containing precursors.

研究领域: 材料科学 · 化学
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NANO · 2019 · IF 1.293

Femtosecond Laser-Assisted Synthesis of ZnO Nanoparticles in Solvent with Visible Emission for Temperature Sensing

Huanhuan Xu,Lihe Yan,Jinhai Si,Yanmin Xu,Xun Hou

Zinc oxide (ZnO) nanoparticles (NPs) are synthesized by one-step femtosecond laser ablation of zinc powders in n-methyl pyrrolidone (NMP) at room temperature. The as-prepared ZnO NPs are fairly stable, water-soluble and have abundant surface functional groups resulting in a strong fluorescence in the visible region. By further annealing the ZnO NPs in the reacting solvent up to 120 ∘ C, the photoluminescence (PL) intensity of material can be significantly enhanced. Besides, the PL of ZnO NPs can change from blue to green by controlling the annealing temperature. The products exhibit excellent temperature sensing with high temperature sensitivity and a 1.3% change per ∘ C response over a linear temperature sensing range (6–84 ∘ C ) ∘C) in aqueous buffer, which matches well with the physiologically relevant temperatures. Hence, the ZnO nanoparticle system can serve as a promising candidate for practical fluorescent temperatures nanosensors which can be used for accurate temperature monitoring within biological systems.

研究领域: 材料科学 · 生物医学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Inducing exciton dissociation in covalent organic framework by local gradient ionic polarization for enhanced hydrogen peroxide photosynthesis

Ruijuan Bian,Yang Deng,Yang Li,Pengfei Li,Ruoyun Gao,Yali Luo,Jingping Lu,Chunhuang Fan,Lifei Liu,Zhinan Xia,Xu Wu

Covalent organic frameworks (COFs) have emerged as a thriving family in the realm of photocatalysis. However, the high exciton dissociation energy and lack of driving force for carrier transport cannot be disregarded. In this work, we proposed a strategy to enhance the built-in electric field of COFs by fabricating local ionic defect on the skeleton. Specifically, a series of metal-free TAPT-EFIB-X (X = 0, 10, 20, 40) with gradient ionic defect concentration were synthesized, which can evenly induce a reshuffling of the local electronic structure, charge distribution, and dipole polarization, thus promoting exciton dissociation and driving electronic transfer. Moreover, TAPT-EFIB-X were endowed with a cationic skeleton and a strong reduction center formed by bromine anions. Among them, TAPT-EFIB-20 achieves high hydrogen peroxide photosynthesis of 8323 μmol h −1 g cat −1 from O 2 and H 2 O. The results show that the strong electron-deficient feature of the TAPT-EFIB-20 promotes the directional distribution of electrons, and the polarization attenuates the spatial barrier effect resulted from the introduction of ionic groups. Subsequently the hybridized orbitals formed by N + and C atoms interact with the corresponding orbitals of adsorbed O 2 to promote the 2e - ORR, while the formation of the hole-rich sites facilitate the 4e - WOR pathway for efficient overall photocatalytic H 2 O 2 generation.

研究领域: 材料科学 · 光催化 · 化学工程
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ELECTROCHIMICA ACTA · 2014 · IF 4.086

Facile one-pot and rapid synthesis of surfactant-free Au-reduced graphene oxide nanocomposite for trace arsenic (III) detection

Wei-Wei Li,Fen-Ying Kong,Jing-Yi Wang,Zhi-Dong Chen,Hai-Lin Fang,Wei Wang

A very simple and effective approach of fabricating Au-reduced graphene oxide (Au-RGO) nanocomposite is herein reported. The nanocomposite was synthesized through a one-pot in situ reduction of graphene oxide (GO) and HAuCl 4 under ultraviolet (UV) irradiation without using any additional chemical reducing agents, capping agents, stabilizer or surfactant. The surface characterization with various techniques such as UV–vis spectroscopy, Fourier transform infrared spectroscopy, Raman spectroscopy and transmission electron microscopy (TEM) showed that GO was effectively reduced and Au nanoparticles with a uniform size were well dispersed on the surface of RGO. This UV light assisted synthesis of Au-RGO nanocomposite is expected to be a universal and clean approach for the formation of various RGO-based nanocomposites. Significantly, the as-prepared nanocomposite possessed high activity in the redox behavior of As (III). Based on the Au-RGO nanocomposite modified electrode , a simple, sensitivity and selective sensing platform for the detection of As (III) was developed. Under optimum conditions, a detection range of 0.3–20   ppb and a low detection limit of 0.1   ppb were obtained, which is found to be well below the World Health Organization (WHO) guidelines of 10   ppb.

研究领域: 材料科学 · 环境科学 · 分析化学
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Journal of Materials Chemistry C · 2018 ·Vol. 6 ·期 43 ·11651-11658 · IF 5.976

Preparation of controllable-thickness 1T@2H-MoS2 thin films by pulsed laser-induced synthesis and the selective separation of the 1T phase

Yishuo Hu,Xiangbin Zeng,Tingting Ren,Shaoxiong Wu,Wenzhao Wang,Yang Zeng,Guangtong Zhou,Zhenyu Guo,Wen Jin,Shibo Wang,Yonghong Xiao,Jingjing Lu

Ultrathin 1T@2H-MoS2 films have excellent electronic and optical properties, and are potentially applicable in optics, electronics, energy storage, and sensing technology. However, identification of an efficient method to produce 1T@2H-MoS2 films with controllable thickness is challenging. This study describes the rapid synthesis (5–10 min) of 1T@2H-MoS2 thin films on Si/SiO2 substrates by a novel pulsed laser irradiation method. We verify the photodecomposition reaction model by measuring the UV-Vis absorption spectra of the reactants. The thickness of the synthesized MoS2 film can be controlled by adjusting the concentration of the precursor. Structural characterization confirms that both the 1T and 2H phases exist in the MoS2 film. The 1T phase enhances the conductive behavior of the MoS2 film and induces magnetism. Furthermore, pure 1T-MoS2 can be separated selectively from the MoS2 film under specific operating conditions using pulsed laser-induced synthesis. This approach is suitable for the synthesis of films of MoS2 and other 2D materials, including 1T phase-pure films.

CAS / MDL: 10241-05-1
研究领域: 材料科学 · 光学 · 电子学
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ChemistrySelect · 2022 ·Vol. 7 ·期 45 ·e202204071 · IF 2.307

Synthesis of Ultrafine Platinum Nanocatalysts by Ice-photochemical Method and Their Application in Catalytic Degradation of 4-nitrophenol

Liang Xian,Jing Ma,Wei Li,Yanzhong Yang,Xu Gao,Bei Xi,Xiaoxia Tian

Graphical Under visible light irradiation at low temperature, uniformly dispersed ultrafine platinum(Pt) nanocatalysts was loaded on fullerene (C 60 ) without adding any reducing agent or stabilizing agent, and was effectively used to catalyze the reduction of 4-nitrophenol. The results show that Pt nanoparticles with good catalytic activity can be finally formed under the action of visible light. This green visible light chemical synthesis method is expected to be popularized in the field of catalysis. Here, uniformly dispersed ultrafine platinum nanocatalysts (Pt/C 60 ) were synthesized on C 60 by ice-photochemical method using potassium chloroplatinate (K 2 [PtCl 4 ]) as platinum source under the condition of low temperature, no stabilizer and reducing agent. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and Transmission electron microscopy (TEM) were used to study the composition and morphology of Pt/C 60 catalyst. It was confirmed that Pt Ultra-small Particles (Pt UPs) was loaded on C 60 surface with high dispersion. The average particle sizes of the three samples obtained under different reaction conditions were 1.41±0.1 nm, 1.54±0.4 nm and 1.73±0.3 nm, respectively. The results show that the light-induced effect and the ice lattice domain limiting effect in the frozen state effectively control the formation and growth of platinum clusters in the process of Pt 2+ reduction to Pt 0 . The rate constants of the three samples were 0.89 min −1 , 0.31 min −1 , 0.19 min −1 , respectively, showing high catalytic activity in the study of the catalytic performance of Pt/C 60 degradation of 4-nitrophenol (4-NP) by Ultraviolet-visible spectroscopy (UV-Vis). This method provides a meaningful attempt for the study of green chemical synthesis method of platinum metal catalysts.

研究领域: 催化材料 · 环境科学 · 纳米技术
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ADVANCED FUNCTIONAL MATERIALS · 2020 ·Vol. 30 ·期 35 ·2001478 · IF 16.836

In Situ Photosynthesis of an MAPbI3/CoP Hybrid Heterojunction for Efficient Photocatalytic Hydrogen Evolution

Cheng Cai,Yuan Teng,Jian-Hao Wu,Jun-Yan Li,Hong-Yan Chen,Jing-Hua Chen,Dai-Bin Kuang

Halide perovskite like methylammonium lead iodide perovskite (MAPbI 3 ) with its prominent optoelectronic properties has triggered substantial concerns in photocatalytic H 2 evolution. In this work, to attain preferable photocatalytic performance, a MAPbI 3 /cobalt phosphide (CoP) hybrid heterojunction is constructed by a facile in situ photosynthesis approach. Systematic investigations reveal that the CoP nanoparticle can work as co-catalyst to not only extract photogenerated electrons effectively from MAPbI 3 to improve the photoinduced charge separation, but also facilitate the interfacial catalytic reaction. As a result, the as-achieved MAPbI 3 /CoP hybrid displays a superior H 2 evolution rate of 785.9 µmol h −1 g −1 in hydroiodic acid solution within 3 h, which is ≈8.0 times higher than that of pristine MAPbI 3 . Furthermore, the H 2 evolution rate of MAPbI 3 /CoP hybrid can reach 2087.5 µmol h −1 g −1 when the photocatalytic reaction time reaches 27 h. This study employs a facile in situ photosynthesis strategy to deposit the metal phosphide co-catalyst on halide perovskite nanocrystals to conduct photocatalytic H 2 evolution reaction, which may stimulate the intensive investigation of perovskite/co-catalyst hybrid systems for future photocatalytic applications.

研究领域: 材料科学 · 光化学 · 催化 · 能源材料
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Catalysis Science & Technology · 2024 · IF 4.4

A diacetylene covalent organic framework through a one-step two-electron O2 reduction pathway for efficient photosynthesis of H2O2

Pengken Li,Hui Zhao,Rong Ji,Wenwen Chi,Xinyu Sun,Yuming Dong,Yongfa Zhu

A one-step two-electron oxygen reduction pathway is crucial for the stable and efficient photosynthesis of hydrogen peroxide. However, the lower oxygen adsorption and activation capacity significantly restrict the ability of the one-step two-electron oxygen reduction pathway. In this work, a covalent organic framework containing a diacetylene unit (COF-Tfp-BDDA) as an efficient oxygen reduction active site was designed for the photosynthesis of hydrogen peroxide. This work demonstrates that the introduction of the diacetylene unit efficiently improved the oxygen adsorption and activation capacity of the COF. Additionally, the introduction of a diacetylene unit effectively promoted charge separation. COF-Tfp-BDDA exhibited a superior rate of H2O2 preparation (880 μmol g−1 h−1) under visible light irradiation from pure water and oxygen, better than most COF-based photocatalysts. The catalyst exhibited a stable hydrogen peroxide photosynthesis efficiency above 100 hours in cycling experiments. Based on the experimental and DFT calculation results, the introduction of a diacetylene unit not only enhances the adsorption and activation of oxygen but also alters the reduction pathway of oxygen, leading to effective charge separation. These factors contribute to the efficient photosynthesis of hydrogen peroxide in pure water. This work provides a novel idea regarding the application of COFs in the field of solar energy conversion.

CAS / MDL: 92-87-5
研究领域: 材料科学 · 光催化 · 太阳能转化
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