Catalysts
·
2025
·Vol. 15
·期 11
·1032
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IF 4
Jingmo Zhou,Chaoyue Liu,Wenke Zhao,Faizan Ahmad,Yaning Zhang
This study pioneers the application of metal-doped Fe-Al as multifunctional redox catalysts for tunable syngas production from plastics via a microwave-assisted process (CLG). We rationally designed a series of redox catalysts (Ni, Ca, Ce, Sr, Co) to unlock efficient H2-rich syngas production from (high-density polyethylene) HDPE. A class of metal-doping (Ni, Ca, Ce, Sr, and Co) Fe-Al redox catalysts was engineered, with Ni-doped Fe-Al (Ni-Fe-Al) exhibiting the excellent H2-rich syngas production (75.32 mmol/gHDPE syngas, 47.09 mmol/gHDPE H2). This is attributed to the improved redox activity, which facilitates efficient lattice oxygen transfer and catalytic reforming reactions, alongside improved microwave absorption and a porous structure that promotes reactant access. This strategic material design, coupled with process parameter optimization (800 W, redox catalyst/plastic = 2.0), developed a highly efficient HDPE-to-syngas conversion system. The process produced a high-quality syngas (90.03% H2+ CO, H2/CO ratio = 2.27) with a rapid heating rate (233.0 °C/min) and minimal energy input (3.52 kWh/molgas). This work provides not just an effective upcycling route for plastics, but a fundamental blueprint for designing advanced redox catalysts to unlock the full potential of microwave-CLG.
研究领域:
催化化学
·
能源工程
·
环境科学
·
材料科学
·
化学工程
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DOI
高影响因子
Nanoscale
·
2025
·
IF 5.1
Shenglong Wu,Lixiong Du,Yajing Wang,Kui Shen,Liyu Chen,Yingwei Li
The reverse water-gas shift (RWGS) reaction provides an important pathway for converting CO2 to CO, which can then be used to produce high-value chemicals through Fischer-Tropsch synthesis. Metal oxide materials, especially Fe2O3, offer considerable potential for use in RWGS reaction at high temperatures, but their catalytic performance is hindered by the inadequate activation and dissociation capabilities of H2 at low temperatures. Herein, we report the introduction of Fe4 with high H2 activation capability near Fe2O3, which shows a synergistic effect and achieves excellent activity and selectivity in RWGS reaction at low temperatures. Fe2O3 nanoparticles and Fe4 clusters supported on carbon (Fe2O3-Fe4/C) were prepared by KCl-assisted pyrolysis of NH2-MIL-88B(Fe) precursors. Fe2O3-Fe4/C delivers a remarkable CO selectivity of 99.4% and a space-time yield of 15.2 μmolCO gcat−1 s−1 at 350 °C and atmospheric pressure. In situ diffuse reflection infrared Fourier-transform spectra and density functional theory calculations demonstrate that the introduction of Fe4 clusters can activate H2 and significantly lower the reaction energy barrier of CO2 hydrogenation on Fe2O3 sites, thus boosting the RWGS performance at low temperatures.
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DOI
PubMed
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2025
·
IF 10.3
Weixia Wang,Yongji Zhang,Fei Zhao,Libo Wang,Fanpeng Meng,Shuchao Qin,Jinsheng Zhao
Carrier recombination in polymer photocatalysts involves both undissociated exciton decay and charge recombination, which are the main obstacles limiting their photocatalytic activity. Achieving efficient charge generation and separation in a polymer system is a fundamental strategy for the potential success of solar energy conversion to hydrogen, but it remains a huge challenge. In this study, we propose an innovative intermolecular π–π stacking strategy to construct a π-delocalized all-polymer S-scheme heterojunction for photocatalytic hydrogen evolution. Two conjugated porous polymers (CPPs)—PyB, composed of benzo[1,2-b:4,5-b′]dithiophene (BDT) and pyrene units, and PhB, composed of BDT and benzene—were synthesized and integrated with CN nanosheets. The highly planar and π-extended structure of PyB facilitated strong interfacial π–π stacking with CN, forming an extended π-delocalized network that enhanced the internal electric field (IEF), improved charge separation, and boosted visible-light absorption. As a result, the optimized PyB/CN-20 composite achieved a remarkable hydrogen evolution rate (HER) of 23.84 mmol⋅h −1 ⋅g −1 under visible light, approximately 287 times higher than that of pristine CN. This work underscores the critical role of polymer planarity and π-conjugation in heterojunction efficiency, and provides new insights into the rational design of π-delocalized S-scheme systems and establishes a general strategy for developing highly efficient, metal-free photocatalysts by leveraging molecular-level structural control.
研究领域:
材料化学
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光催化
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高分子科学
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能源材料
·
纳米材料
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物理化学
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太阳能转换
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Shikai Wang,Dong Zhang,Dafeng Zhang,Xipeng Pu,Junchang Liu,Hengshuai Li,Peiqing Cai
Reasonable design of high-performance catalysts with heterojunction to suppress the combination of electron-hole pairs has become an appealing challenge in photocatalytic field. Herein, a novel hydrangea-like ZnIn 2 S 4 /FePO 4 with S-scheme heterojunction was constructed via an ultrasound-annealing process for photocatalytic H 2 evolution. The composites showed remarkable photocatalytic H 2 production performance (3.337 mmol h −1 g −1 ), which was approximately 7.5 times higher than that of blank ZnIn 2 S 4 (0.446 mmol h −1 g −1 ). The improved photocatalytic H 2 evolution was mainly ascribed to the accelerated electron-hole separation through the construction of S-scheme heterojunction in interface. Moreover, the hydrangea-like structure provided abundant active sites and huge specific surface area, which was conducive to the exceptional photocatalytic activity. Simultaneously, both experimental and Density Functional Theoretical calculation results provided strong evidence for the transfer path of photogenerated carriers following the S-scheme heterojunction, and the unique mechanism of photocatalytic H 2 production was proposed. In addition, the hydrangea-like ZnIn 2 S 4 /FePO 4 heterojunction photocatalyst showed a commendable stability with no distinct decrease after three cycle tests, demonstrating its potential as a recoverable photocatalyst. This work offered insights into the design and preparation of highly efficient photocatalysts with S-scheme heterojunction.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2022
·
IF 0.847
Ruiqi Gao,Huan He,Junxian Bai,Lei Hao,Rongchen Shen,Peng Zhang,Youji Li,Xin Li
ABSTRACT Nowadays, conjugated polymers have garnered numerous attention as a new class of organic photocatalysts due to their tunable electronic properties, low cost, excellent stability and sufficient light-absorption performance. In particular, pyrene-benzothiadiazole-based conjugated polymer (PBBP) has been considered to be a new type of conjugated polymers for photocatalytic H 2 evolution. However, the poor charge separation seriously limits its practical application in H 2 evolution. In this work, a PBBP-based polymer/CdS 2D/2D organic/inorganic S-scheme heterojunction photocatalyst with a strong internal electric field is, for the first time, prepared for efficient photocatalytic hydrogen evolution. The pyrene-benzothiadiazole-based conjugated polymers (PBBP) are synthesized by the Suzuki-Miyaura reactions. Then, the hybrid heterojunction photocatalysts are fabricated by coupling CdS with it through the ultrasonic mixing method. As a result, the highest H 2 -production rate of 15.83 mmol h −1 g −1 is achieved on 20% PBBP/CdS composite under visible-light irradiation, nearly 2.7 times higher than that of pure CdS. The apparent quantum efficiency (AQE) of 20% PBBP/CdS composite could reach 8.66% at λ = 420 nm. The enhanced activity could be attributed to the construction of S-scheme heterojunction, which accelerates the recombination of carriers with weaker redox ability and maintains the strong reducibility of electrons in CdS. This work provides a protocol for pyrene-benzothiadiazole-based conjugated polymers to prepare S-scheme heterojunction photocatalysts based on organic/inorganic coupling.
研究领域:
材料科学
·
化学工程
·
光化学
·
催化
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Zaiyong Yang,Zhiheng Hao,Shunxin Zhou,Peng Xie,Zengxi Wei,Shuangliang Zhao,Fuzhong Gong
Direct synthesis of hydrogen peroxide (DSHP) from H2 and O2 offers a promising alternative to the present commercial anthraquinone method, but it still faces the challenges of low H2O2 productivity, low stability of catalysts, and high risk of explosion. Herein, by loading in a microchannel reactor, the as-synthesized Pd–Sn alloy materials exhibit high catalytic activity for H2O2 production, presenting a H2O2 productivity of 3124 g kgPd–1 h–1. The doped Sn atoms on the surface of Pd not only facilitate the release of H2O2 but also effectively slow down the deactivation of catalysts. Theoretical calculations demonstrate that the Pd–Sn alloy surface has the property of antihydrogen poisoning, showing higher activity and stability than pure Pd catalysts. The deactivation mechanism of the catalyst was elucidated, and the online reactivation method was developed. In addition, we show that the long-life Pd–Sn alloy catalyst can be achieved by supplying an intermittent flow of hydrogen gas. This work provides guidance on how to prepare high performance and stable Pd–Sn alloy catalysts for the continuous and direct synthesis of H2O2.
研究领域:
化学工程
·
催化科学
·
材料科学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Qingping Wu,Yao Cheng,Feng Huang,Xiao Li,Xiangshui Cui,Ju Xu,Yuansheng Wang
Atomic defects (e.g., Ti 3+ , oxygen vacancies) have been intenstively investigated for modifying TiO 2 in order to reach visible light active photocatalytic H 2 production. However, the atomic defects within TiO 2 could easily act as photo-generated charge-carrier recombination centers, resulting in relatively low H 2 conversion efficiency. In this paper, semicrystalline yellow TiO 2 nanoparticles rich of superoxide ions are new synthesized by a simple aqueous solution method. Instead of introducing atomic defects, we show for the first time that catalytic performance can also be significantly improved via in-situ creating lattice O O bonds within metastable semicrystalline TiO 2 . The synthesized semicrystalline yellow TiO 2 exhibits significantly enhanced photocatalytic activity for H 2 production after cycle tests. The formaldehyde in aqueous solution is used as target pollutant to simulate industrial wastewater. In-situ created elastic lattice O O bonds are proposed to improve catalytic performance through facilitating the breakage of C H bonds of HCHO. A series of internally consistent reaction equations is proposed that describes the role of in-situ created lattice O O bonds for improving the catalytic performance. This is strongly supported by that the H 2 production rate at the end of the fourth cycle test is significantly more than that of the beginning of the first cycle test.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Wanbing Gong,Chun Chen,Yong Zhang,Hongjian Zhou,Huimin Wang,Haimin Zhang,Yunxia Zhang,Guozhong Wang,Huijun Zhao
A copper-based catalyst, which was supported by sulfonate group (−SO3H) grafted active carbon (AC), was prepared and activated simultaneously by liquid phase chemical reduction method. The modified copper catalyst, Cu/AC–SO3H, displayed an enhanced catalytic performance for selective hydrogenation of furfural (FAL) to furfuryl alcohol (FOL) in liquid phase, in which almost 100% FOL yield was obtained at 378 K and 0.4 MPa of hydrogen pressure after 120 min reaction. The effect of −SO3H was evaluated and illustrated by the combination of reaction performance and physicochemical characterizations, such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectrometer (XPS) measurements. Through grafting sulfonate group on the support, better dispersion of nanoparticles, higher reduction degree of Cu, and stronger adsorption of FAL can be attained to contribute high hydrogenation performance. In addition, the effects of reaction conditions (such as reaction temperature, H2 pressure, reaction time, solvent, and catalyst to FAL mass ratio) were evaluated intensively. Also, the Cu/AC–SO3H catalyst showed an excellent catalytic performance for transfer hydrogenation of FAL, in which 2-propanol was utilized as the solvent and hydrogen donor concurrently. Cycling test proved the prepared catalyst could be recycled and reused for several times without noticeably reduced catalytic activity of hydrogenation.
研究领域:
化学工程
·
催化科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Shumin Li,Jun Tan,Zhejun Jiang,Jin Wang,Zhengquan Li
Dye-sensitized systems show promising in photocatalysis because they can separate the tasks of light absorption, charge generation and surface catalysis to two coupled components. In this system, it is crucial to develop suitable catalysts capable of receiving dye-injected charges and having high activity to a given reaction. Aiming to photocatalytic H 2 and O 2 production, we present a metal-organic framework derived route to prepare bimetallic Fe-Ni-P nanotubes using Fe-Ni-MIL-88 nanorods as templates. When integrated with different dyes, these Fe-Ni-P nanotubes can serve as efficient catalysts for photocatalytic H 2 and O 2 production, respectively. Additionally, catalytic activities of such dye-sensitized systems can be conveniently regulated by tailoring the metal compositions in Fe-Ni-P nanotubes. The photocatalytic H 2 production of Fe 1 -Ni 2 -P can reach 5420 μmol g cat −1 h −1 under eosin-Y sensitization, which is 24 times and 6.7 times higher than Fe 2 P and Ni 2 P, respectively. The photocatalytic O 2 production of Fe 1 -Ni 2 -P can reach 900.3 μmol g cat −1 h −1 under [Ru(bpy) 3 ]Cl 2 sensitization, about 4.6 times and 2.9 times higher than Fe 2 P and Ni 2 P. The roles of different components in the system have been explored and corresponding working mechanism is proposed. This work demonstrates a new type of dye-sensitized systems consisting of bimetallic phosphides and provides a facile route to regulate their photocatalytic performance.
研究领域:
材料科学
·
光催化
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DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Tawanda Matamba,Arash Tahmasebi,Salman Khoshk Rish,Jianglong Yu
This study reports the role of pressure (0.1–4.0 MPa) and temperature (600–900 °C) in flash pyrolysis of palm kernel shell (PKS). The main objective was to study the extent to which pressure affects the mechanism of pyrolysis reactions to enhance the selective production of target products. Higher pressures and temperatures selectively promoted the generation of polycyclic aromatic hydrocarbons (PAHs) and H2 gas. Bio-oil samples generated at lower temperatures and pressures were mainly composed of phenolics. Increasing the pressure and temperature favored the selective formation of phenanthrene, fluoranthene, pyrene, fluoranthene, and fluorene, which reached 96.17 area %. Elevated temperatures and pressures enhanced hydrogen transfer into a light gaseous phase. The yield of H2 peaked at 40.82 g of H2/kg of PKS at 900 °C and 2.0 MPa. The results obtained in this study implied that the pyrolysis of biomass at elevated pressures can be an effective method for polygeneration of hydrogen gas and PAHs as chemical feedstocks.
研究领域:
能源科学
·
环境科学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Hao Guo,Jiaqin Liu,Yanhong Li,Jürgen Caro,Aisheng Huang
Due to their rationally controlled pore size and easy functionalization, metal-organic frameworks (MOFs) are a promising candidate for membrane separation . As one of the most stable MOFs, UiO-66 has attracted intense attention for the preparation of molecular sieving membranes. A new post-synthesis modification (PSM) strategy was developed to enhance the separation selectivity of supported UiO-66-NH 2 membranes on porous ceramic tubes called UiO-66-NH 2 @SA by using salicylaldehyde (SA) modification. The mixed gas separation factors of H 2 /CO 2 and H 2 /CH 4 can be improved due to constrictions of the pore size through reaction of –NH 2 with SA giving iminophenol moieties. Notably, SA-modified UiO-66-NH 2 membranes are rather stable, at a high operation temperature of 200 °C and 1 bar, mixture separation factors of 11.3 for H 2 /CO 2 and 22 for H 2 /CH 4 can be obtained. Further, no obvious performance degradation has been observed after 3 months storing in air. This high stability of UiO-66-NH 2 @SA membrane could provide possibility for the industrial applications of hydrogen separation and purification.
研究领域:
材料科学
·
化学工程
·
膜技术
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Mengli Han,Peng Gao,Jianhai Wang,Yuesong Shen
While noble metal single atoms (SAs)/semiconductor photocatalysts offer outstanding catalytic performance, challenges related to dosage and stability limit their broader application. In this study, we present a controlled photoreduction strategy that leverages synergistic photoreduction conditions, steric hindrance, and complexation to significantly enhance both activity and stability with an ultra-low Pt loading. The optimized Pt/TiO 2 catalyst (0.0063 wt% Pt) exhibits a 73-fold increase in photocatalytic activity, achieving a Pt mass activity of 6.24 mol/g/h. XPS analysis and DFT calculations reveal that Pt atoms are deposited on TiO 2 via strong interactions resembling an O-Pt-O bond, effectively preventing the migration and aggregation of highly dispersed Pt SAs, thereby significantly improving catalyst stability. Additionally, the ΔG H * for Pt 2+ SAs is nearly 0 (−0.002 eV), enabling rapid H adsorption and H 2 desorption, which imparts the catalyst with exceptional catalytic performance. This study paves the way for the development of catalysts with minimal precious metal content, enhanced efficiency, and extended stability.
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DOI
高影响因子
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