SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Yong Guo,Xudong Miao,Xueyang Zhang,Huinan Che,Ying Li
The development of novel metal-free catalysts to photosynthesize hydrogen peroxide (H 2 O 2 ) is recognized as a prospective technology for sustainable energy conversion. Herein, the carbon-doped boron nitride (BCN) and perylene tetracarboxylic dianhydride (PTCDA) formed PDA@BCN S-scheme heterojunctions with π-π stacking, which catalyzed the production of H 2 O 2 at an unexpectedly high yield of 285.47 μmol h −1 g −1 in air. The high photocatalytic performance is attributed to the enhanced light absorption resulting in abundant carrier excitation, rapid charge separation driven by S-scheme heterojunctions, and highly selective H 2 O 2 formation pathway. Theoretical calculations demonstrate that carbon sites in PDA@BCN can serve as an advanced active center for oxygen enrichment and activation, promoting oxygen reduction and efficient photocatalytic production of H 2 O 2 . This work lays the foundation for the design of efficient, stable, and reusable photocatalysts for environmental restoration and energy conversion.
研究领域:
材料科学
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光化学
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环境科学
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Xintong Zhou,Chang-jun Liu
Structured porous carbon materials have been extensively applied for catalyst, sensor, adsorbent, energy storage materials and many others. However, the preparation of such carbon materials in a controllable way remains a significant challenge. In this work, 3D printing has been employed to prepare porous carbon structures with tailorable pore sizes. A starch/gelatin ink has been applied as carbon source with SiO 2 monodispersed spheres as hard template. The process exhibits an excellent printing accuracy. Controllable meso and macro structures can be thereby obtained. The printed monolithic structures have been used as metal-free catalysts for the selective oxidation of benzyl alcohol, as an illustration. The monolithic and meso/macro-porous structure has a remarkable influence on the reaction rate. A high conversion with high benzaldehyde selectivity has been achieved. The 3D printing strategy provides us a simple, low cost and reliable way of fabricating carbon structures with designable meso/macro-pores, which is promising for many other applications beyond catalysis.
研究领域:
材料科学
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催化化学
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能源材料
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纳米结构材料
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功能材料
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
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2016
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IF 6.333
Hui Wu,Liang Shi,Jiaheng Lei,Dan Liu,Deyu Qu,Zhizhong Xie,Xiaodi Du,Peng Yang,Xiaosong Hu,Junsheng Li,Haolin Tang
The development of efficient and durable catalyst for oxygen reduction reaction (ORR) is critical for the practical application of proton exchange membrane fuel cell (PEMFC). A novel imidazole based ionic liquid is synthesized in this study and used subsequently for the preparation of a N and S co-doped metal-free catalyst with three dimensional ordered microstructure. The catalyst prepared at 1100 °C showed improved ORR catalytic performance and stability compared to commercial Pt/C catalyst. We demonstrate that the high graphitic N content and high degree of graphitization of the synthesized catalyst is responsible for its superb ORR activity. Our results suggest that the N and S co-doped metal-free catalyst reported here is a promising alternative to traditional ORR catalyst based on noble metal. Furthermore, the current study also demonstrate that importance of morphology engineering in the development of high performance ORR catalyst.
研究领域:
电催化
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能源材料
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纳米材料
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物理化学
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燃料电池
✓ 已验证
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 55
·44128-44136
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IF 3.84
Yufang Tao,Qian Ni,Mingyu Wei,Dongsheng Xia,Xiaoxia Li,Aihua Xu
Semiconducting carbon nitride materials (g-C3N4) were investigated as metal-free catalysts for the activation of peroxymonosulfate (PMS) under visible light irradiation to degrade organic dyes in aqueous solution. X-ray diffraction, scanning electron microscopy, N2 adsorption/desorption isotherms, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy were used to characterize the properties of the material. The effect of several parameters including the concentration of catalyst, PMS and organic dye, and initial solution pH on its catalytic activity was also investigated. It was found that the obtained g-C3N4 can effectively activate PMS under visible light irradiation to generate strong sulfate radicals which was highly active for Acid Orange 7 (AO7) and other organic dyes degradation. The catalyst also presented a long-term stability during multiple runs. Based on intermediate detections, the degradation pathway of AO7 in the g-C3N4/PMS/Vis system was proposed. This study demonstrated a promising approach for the activation of green oxidant, PMS, by the newly-developed polymer photocatalysts for environmental remediation and oxidation catalysis.
研究领域:
环境化学
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光催化
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材料科学
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水处理技术
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氧化催化
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纳米材料
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Kaiqiang Wei,Haodong Nie,Yi Li,Xiao Wang,Yan Liu,Yajie Zhao,Hong Shi,Hui Huang,Yang Liu,Zhenhui Kang
Artificial photoproduction of hydrogen peroxide (H 2 O 2 ) from H 2 O and O 2 by metal-free catalysts (e.g., graphitic carbon nitride) is regarded as an ultra-clean approach. Metal-free catalysts are often hindered by unpropitious rapid charge recombination and unfavorable selectivity. Herein, three carbon dots (CDs1 to CDs3) decorated modified-carbon nitride (CDs1-NCN, CDs2-NCN and CDs3-NCN) were designed and fabricated, which show diverse activity of H 2 O 2 photoproduction. Among them, CDs1-NCN, as a two-channel photocatalyst, achieves H 2 O 2 production with high efficiency (1938 μmol h −1 g −1 ). This process is at normal pressure and without sacrificial agent under visible region ( λ ≥ 420 n m ) , which is 27.5- times higher than that of pristine C 3 N 4 . The apparent quantum efficiency can be calculated to 7.03 % ( λ = 365 n m ) . In this system, CDs with different energy levels dominate the activity of metal-free catalyst for hydrogen peroxide photoproduction. Combining with photoelectrochemical test and transient photovoltage analysis, the active site and the catalytic mechanism of these composite catalysts are also clarified. Our work provides a clearly insight for understanding of the regulation of interfacial electron transport in metal-free photocatalysts.
研究领域:
材料科学
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化学
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催化
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光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Biochar
·
2023
·Vol. 5
·期 1
·1-18
·
IF 12.7
Wang Shulian,Huang Yan,Ma Shuanglong,Zhan Sihui,Wang Jingzhen,Gao Boqiang,Tang Xiaodan,Zhu Qiuhui,Xu Shengjun,Zhuang Xuliang
Metal-free porous biochars are popularly utilized as catalysts for peroxydisulfate (PDS) activation. The enhancement effect of PDS activation of porous biochars fabricated by employing both hard template and alkali metal activating agent has not been explored completely. In addition, the role of the inherent carbon defect in PDS activation has not been clearly elucidated. Hence, a series of carbonaceous catalysts were fabricated using a sole template (KCl), a sole activating agent (Na 2 S 2 O 3 ) or a combination of template and activating agent (KCl/Na 2 S 2 O 3 , KCl/KHCO 3 , KCl/NaHCO 3 , and KCl/Na 2 C 2 O 4 ), to systematically investigate the effect of specific surface area (SSA) and intrinsic defect of porous biochar on its PDS activation ability. The biochar synthesized by KCl and Na 2 S 2 O 3 (SK-C) exhibited the optimum degradation performance. The SK-C was found to possess an interconnected hollow cage with three-dimensional mesh structure showing the largest surface area, pore volume and C- sp 3 edge defect content among all the catalysts, which explained its paramount catalytic ability. The SSA and C- sp 3 content together can determine the catalytic performance in a quantitative relationship. The single electron transfer pathway from SDZ to inner-sphere bound SK-C/PDS* was the protagonist of pollutant oxidation. The degradation intermediates were detected and recognized and their toxicities were evaluated. This study for the first time comprehensively identified the synergistic effect between the SSA and inherent defects on improving the catalytic performance of biochar for PDS activation to removal contaminants. Graphical Abstract
研究领域:
环境科学
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材料科学
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化学工程
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水处理
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xingrui Gao,Xiao Liu,Xixi Di,Yixuan Shi,Dong Liu,Jingxi Yang,Zuoping Zhao,Wei Wang,Xiaohui Ji,Xianzhao Shao
Environmentally friendly advanced oxidation (AOPs) is an effective means to treat trace amounts of antibiotics in water. However, traditional transition metal catalysts face challenges of metal leaching, limiting their practical utility. In this research, by activating peroxymonosulphate (PMS) using a nitrogen-phosphorus co-doped porous carbon (NP-HPMC-900) catalyst, a non-radical-dominated degradation mechanism was achieved. Material characterization revealed uniform distribution of N (3.35 at%) and P (2.56 at%) dopants in NP-HPMC-900, significantly enhancing the electronic structure and defect density ( I D /I G = 0.86) of the carbon framework. Catalytic degradation experiments demonstrated that NP-HPMC-900 achieved 90 % tetracycline hydrochloride (TCH) removal within 30 min at pH 4, 6 and 10, with a superior apparent speed constant ( k obs = 0.02671 min −1 ) compared to conventional metal-based catalysts. Density functional theory (DFT) calculations confirmed that N-P doping modulated the local electron density of carbon matrix, enhancing its electron donor properties and PMS activation capability. Ecological toxicity assessments revealed significantly reduced phytotoxicity of degradation products, validating environmental safety. This study proposes a general strategy for activating PMS through N-P co-doped carbon materials from the perspective of catalyst-PMS synergistic degradation of pollutants, providing theoretical and practical insights into metal-free catalysts for sustainable water treatment.
研究领域:
环境科学
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水处理
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高级氧化工艺
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材料科学
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催化
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毒理学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Materials Advances
·
2022
·Vol. 3
·期 10
·4243-4251
·
IF 0
Qiang Hong,Qingyao Wu,Zhenyu Wu,Yan Liu,Yi Li,Hui Huang,Yang Liu,Zhenhui Kang
Metal-free polymer-based catalysts have shown promising photocatalytic performance for efficient hydrogen peroxide (H2O2) photoproduction under visible light. However, the structure of the active site and the interface charge transfer of these catalysts have not been revealed clearly. Here, we report the fabrication of four narrow bandgap single-dye-based polymer metal-free catalysts (PPC-X, X = 75, 100, 125, 175). The catalyst PPC-X was synthesized by a hydrothermal method using proanthocyanidin (OPC) as the raw material. The reaction temperature was set at 75 °C, 100 °C, 125 °C, and 175 °C, and finally, the single-dye polymer catalyst was obtained, which was marked as PPC-X, with X representing the polymerization temperature. The PPC-X as catalysts show diverse catalytic behavior for H2O2 photoproduction. Under visible light excitation, the PPC-X catalysts (X = 100, 125, 175) reduced O2 to produce H2O2via the two-electron transfer pathway and oxidized water to release O2 by the four-electron transfer pathway. For the PPC-75 catalyst, O2 was reduced by photo-generated electrons on the catalyst surface via the two-electron transfer pathway, while the PPC-75 catalyst itself also serves as a sacrificial agent to consume the photo-generated holes, leading to a high H2O2 production. The H2O2 yield of PPC-75 is 1152 μmol g−1 h−1, and that of PPC-100 is up to 1214 μmol g−1 h−1 at a light intensity of 32.6 mW cm−2. This work provides a practical research example and idea for the in-depth understanding and design of efficient polymer-based photocatalysts.
研究领域:
材料科学
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化学
·
催化
·
光化学
✓ 已验证
产品关联
DOI
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Guoping Pan,Jia Wei,Mengdie Xu,Jiamei Li,Linhao Wang,Yanan Li,Nan Cui,Jun Li,Zhaoxu Wang
In recent years, metal-free catalysts for persulfate-mediated oxidation processes have been widely applied to remove contaminants in the aquatic environment. Herein, a simple pyrolysis approach was used to synthesize the boron doped biochars (B@TBCs) derived from boric acid mixed with tea seed shells powders. The obtained B@TBCs exhibited fantastic capability to boost PMS (0.5 mM) activation for 90%∼ removal of oxytetracycline (OTC) within 20 min. Through the correlation analysis and DFT calculations, it was concluded that the apparent rate constant of pollutants removal was greatly related to the -O-B-O- groups on the biochars, which could improve the electron-donating capacity of the biochar. In addition, the degradation process of OTC was pH-dependent because of the changed roles of ROSs under different pH. Finally, according to the DFT calculation, LC-MS and toxicological analysis, the degradation pathways of pollutants and the toxicity changes during the degradation process were obtained. These findings consolidated the theoretical basis for further boosting the catalytic activity of B-doped biochars and expanded the imagination for the modification of other metal-free biochar catalysts for PMS activation .
研究领域:
环境科学
·
催化
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yan Zhang,HuiYi Pan,Mengru Wang,Xiying Li,Guifeng Lu
Carbon-based composites, especially for heteroatom incorporation including P, S, N, and B, show excellent performance in the ORR and are promising alternatives in place of Pt/C catalysts. However, complex procedures are necessary for the synthesis of the precursors acting as suitable carbon-based electrocatalysts. Herein, a simple method, based on the Schiff-base reaction, offering the privileges of devising the N-containing precursors, is developed to synthesize an efficient ORR catalyst. In this study, a Schiff-base polymer with nanoflower morphology (CNF-P) is synthesized via the reaction of 3,5-diaminobenzoic acid and terephthalaldehyde at room temperature. Subsequently, the N/S-codoped carbonaceous nanoflower electrocatalyst derived from its polymer counterpart (N/S-CNF900) is fabricated through high-temperature pyrolysis of CNF-P with thiourea. Benefitting from the dopants of N and S atoms, the N/S-CNF900 sample demonstrates exceptional ORR activity, offering an E1/2 of 0.87 V, Eonset of 1.02 V, and jm of 6.05 mA cm–2, as well as excellent durability and methanol resistance. When utilized as the air electrode in ZABs, N/S-CNF900 demonstrates superior power output of 178 mW cm–2 coupled with exceptional charge–discharge durability spanning 282 h. The superior electrochemical performance stems from the abundant active sites created by heteroatomic N/S doping with a very high specific surface area and the multilevel porous architecture, thereby ensuring effective exposure of active sites. These findings suggest that the catalyst synthesized through the Schiff-base reaction holds promising potential applications in alkaline zinc–air batteries (ZABs).
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米技术
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Qingyao Wu,Mengmeng Zhu,Jingjing Cao,Xiao Wang,Yang Liu,Chensheng Xiang,Mingwang Shao,He Tian,Zhenhui Kang
Hydrogen can be used as a conventional clean energy resource, only by obtaining it in a cheap, simple, and feasible way. From the perspective of solar energy utilization, photocatalytic water splitting is essentially limited by high electric energy and intermittent solar energy. Here, we demonstrate that the carbon defects could decompose water directly by using low-value mechanical energy in the daily environment without using the sacrificial agent. The prepared metal-free carbon catalyst (OPC-900) with rich graphene topological defects shows several redox states in acetonitrile, which can accumulate redox equivalents and respond for overall water splitting in air at room pressure. Under stirring or light conditions, charges can be created and accumulated on the catalyst surface and split water into H2 and O2 in low conductivity medium. The mechanical energy conversion efficiency of stirring in ultrapure water is 7.01%. Our work combines visible light with low-value mechanical energy for widespread decomposition of water to produce hydrogen in air under normal pressure.
研究领域:
能源材料
·
催化
·
可再生能源
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Ling Ouyang,Qiang Zhou,Jie Liang,Longcheng Zhang,Luchao Yue,Zerong Li,Jun Li,Yongsong Luo,Qian Liu,Na Li,Bo Tang,Abdulmohsen Ali Alshehri,Feng Gong,Xuping Sun
Electrocatalytic NO reduction is a promising technology for ambient NO removal with simultaneous production of highly value-added NH 3 . Herein, we report that honeycomb carbon nanofiber coated on carbon paper acts as an efficient metal-free catalyst for ambient electroreduction of NO to NH 3 . In 0.2 M Na 2 SO 4 solution, such catalyst achieves an NH 3 yield of 22.35 μmol h −1 cm −2 with a high Faradaic efficiency of up to 88.33%. Impressively, it also shows excellent stability for 10-h continuous electrolysis. Theoretical calculations reveal that the most active center of functional groups is –OH group for NO reduction with a low energy barrier (ΔG of 0.29 eV) for the potential-determining step (*NO + H → *HNO).
研究领域:
环境科学
·
材料科学
·
电化学
·
催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）