APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Ge Li,Chunxiao Jin,Baodong Wang,Ziran Ma,Pan Gao,Shuwei Zhou,Renqin Chang,Yuxue Yue,Jia Zhao
The electrochemical NRR, which can be driven by renewable energy sources, is an emerging strategy for addressing the high energy consumption and CO 2 emission issues caused by the traditional Haber–Bosch ammonia synthesis technique. FePc catalyzes the electrochemical ammonia synthesis reaction well, but intermolecular π-stacking and multi-layer overlapping lead to low NH 3 yields. Here, [Bmim][Cl] and [Bmim][NTF 2 ] ILs were used to induce monolayer dispersion of FePc. Ionic-liquid-induced FePc electrocatalyst, namely FePc/C-700, which was constructed with ILs as the carbon source, gave an excellent NH 3 yield (24.25 μg mg cat −1 h −1 ) and Faradaic efficiency (30.59%) at − 0.1 V. The formation of a monolayer FePc structure was confirmed by HAADF-STEM and XANES. The results of DFT calculations and NRR experiments showed that the monolayer FePc structure promoted N 2 adsorption and inhibited the competitive HER. These results will be useful in the design of active sites of layered macromolecules to achieve efficient electrochemical NRR.
研究领域:
材料科学
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电化学
·
催化化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Lulin Wang,Wangyang Lu,Dongjing Ni,Tiefeng Xu,Nan Li,Zhexin Zhu,Haixiang Chen,Wenxing Chen
In the field of environmental catalysis, the construction of highly efficient and stable catalytic oxidation processes has raised considerable attention. In this study, a novel solar-initiated photocatalytic oxidation system, FePcCl 16 /PMS/Sunlight, was established by iron hexadecachlorophthalocyanine (FePcCl 16 ) with peroxymonosulfate (PMS) in the presence of sunlight excitation. Under sunlight irradiation, the phthalocyanine ring of the FePcCl 16 is motivated to FePcCl 16 ∗ in the excited state, which activates PMS to generate free radicals or high–valent iron(IV)-oxo intermediates (Fe(IV) = O) to oxidize carbamazepine (CBZ). The system could degrade CBZ effectively and total-organic-carbon removal from solution reached nearly 80% within 90 min. FePcCl 16 catalytic activity was almost without loss and without iron leaching after twenty recycles, indicating that the FePcCl 16 /PMS/Sunlight was a stable and efficient photocatalytic oxidation system. Electron paramagnetic resonance, gas chromatography-mass spectrometry and photocatalytic-activity-experiment analysis shows that Fe(IV) = O species, singlet oxygen ( 1 O 2 ), hydroxyl and sulfate radicals ( OH, SO 4 − ) are the main active species in the catalytic oxidation of CBZ. Density functional theory (DFT) calculations exhibits that the electronic cloud for excited state FePcCl 16 ∗ is transferred from the porphyrazine ring and peripheral substituents to the central Fe atom and its axial position. The main degradation intermediates and possible degradation pathway of CBZ were proposed by ultra-performance liquid chromatography and high-resolution mass spectrometry (UPLC Synapt G2-S HDMS). This study provides efficient catalytic oxidation support for wastewater treatment.
研究领域:
环境科学
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催化化学
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废水处理
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Hengli Qian,keyuan Zhang,Chao Xie,Qidong Hou,Ruite Lai,Guanjie Yu,Tianliang Xia,Xinyu Bai,Meiting Ju
To achieve efficient degradation of pharmaceuticals and personal care products (PPCPs), the g-C₃N₄-WO₃@FePc system was in-situ constructed using a calcination method, with g-C₃N₄-WO₃ serving as the support matrix. This approach effectively resolved the issue of FePc aggregation and self-degradation in aqueous environments. The g-C₃N₄-WO₃@FePc catalyst demonstrated excellent performance in the photo-Fenton degradation of acetaminophen (ACE), achieving over 90% degradation within just 20 minutes under simulated sunlight. The catalyst's superior performance is attributed to the synergistic effects between the reaction centers. The π-π conjugation between g-C₃N₄-WO₃ (the photocatalytic center) and FePc (the Fenton catalytic center) facilitates the transfer of photo-generated electrons from the photocatalytic center to the Fenton catalytic center, enabling rapid regeneration of Fe(II) and generating a significant amount of active species (•O₂⁻ and 1 O₂). To validate the stability of the catalytic system, factors such as ionic impurities and water types affecting performance were investigated and analyzed. Additionally, cell toxicity and antimicrobial tests were conducted to evaluate the toxicity of ACE degradation intermediates and the ecological stability of g-C₃N₄-WO₃@FePc, revealing its potential for practical wastewater treatment applications.
研究领域:
环境催化
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光化学
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水处理
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材料科学
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环境毒理学
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纳米催化
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污染物降解
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2026
·
IF 4.6
Yu Wang,Danyang Wu,Jiao wu,Xizhen Zhang,Yongze Cao,Baojiu Chen
We breakthrough the conventional high-temperature paradigm for synthesizing transition metal catalysts by discovering 500 °C as a critical metastable window in ultrafast (>1500 °C/s) Joule heating synthesis. This kinetically confined thermal shock at precisely 500 °C uniquely terminates metal aggregation while locking abundant pyridinic-N sites (2.86 at.%) that effectively anchor highly dispersed Fe and Co species, simultaneously sculpting a defect-rich carbon matrix. This unique combination, inaccessible in traditional pyrolysis, unlocks exceptional synergistic activity. Consequently, the 500 °C-engineered NC-FeCo catalyst achieves an oxygen reduction record: half-wave potential (0.92 V) surpassing Pt/C (0.85 V) and 1500 °C-treated analogs (0.85 V), while delivering near-theoretical 4e − selectivity (<1.2% H₂O₂), negligible decay (ΔE = 3 mV/5000 cycles), and superior methanol tolerance. Our work establishes sub-second 500 °C thermal shock as an innovative platform for metastable dual-metal electrocatalysis.
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 21.1
Yinkun Gao,Shuyun Guan,Yongqing Wan,Mingyang Liu,Yiman Ma,Xiaojie Xu,Jiashu Yuan,Guokang Han,Peng Gao,Yongming Zhu,Shuaifeng Lou,Xudong Li
Single-dispersed active sites show great promise for lithium-oxygen batteries (LOBs) due to their unique chemical environments and high utilization rates. However, the inherent limitations of surface orbital steric effects and internal electronic coupling yield a detrimental impact on the stability of the active center, particularly during multipathway transformations and electronic recombination evolution of reaction intermediates. In this work, we introduce a curvature-triggered geometric deformation engineering to enhance the dynamic evolution of adsorption and activation processes for intermediates. By optimizing the dynamic geometric deformation of planar molecules through reasonable substrate strain, the deposition and decomposition kinetics of discharge products via dual growth pathways were facilitated, enabling the development of a highly stable LOBs with an impressive cycle life exceeding 1800 hours. Our research uncovers the multi-dimensional correlations among orbital rehybridization, the depth of electronic structure recombination, and the LiO 2 intermediate adsorption energy landscape under spatial confinement effects, providing valuable insights for their future design and activity promotion.
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Dandan Jiang,Danyang Wu,Yu Wang,Yongze Cao,Xizhen Zhang,Baojiu Chen
The design of Pd-based alloys with tailored electronic structures and stable architectures is crucial for enhancing catalytic properties. Here, we present a rapid Joule heating strategy for fabricating a palladium-iron (PdFe) alloy anchored on nitrogen-doped carbon (NC–FePd) featuring exceptional performance and durability. By combining ultrafast phase formation and quenching, the NC-FePd system achieves uniform dispersion of cubic-phase FePd 3 nanoparticles with minimized agglomeration. X-ray diffraction and XPS analyses reveal lattice expansion planes and electron transfer between Pd and Fe, which lowers the d-band center of Pd, thereby weakening the Pd–O binding energy. In alkaline media, NC-FePd achieves an exceptional half-wave potential (0.84 V vs. RHE), showing a clear advantage over commercial Pt/C (0.82 V vs. RHE), coupled with elevated limiting current density (6.01 mA cm −2 ) and the diminished Tafel slope (53.73 mV dec −1 ). This work sheds light on the synergy between rapid Joule-heating synthesis and Fe–Pd electronic modulation for designing durable alloy catalysts.
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产品关联
DOI
高影响因子
TALANTA
·
2025
·
IF 6.1
Xiaodan Qi,Shengnan Zhang,Zhifei Wang,Han Zhang,Lianghui Ma,Lihua Jin,Yehua Shen
The emerging field of nanozymes has introduced unprecedented opportunities and challenges for activated charcoal materials derived from biomass waste. By incorporating specific nanostructures or elements, it is possible to overcome the limitations of traditional activated charcoal, such as insufficient catalytic active sites and poor electron transfer efficiency, thereby unlocking its full potential for various applications. In this study, we successfully synthesized trace Fe-doped activated charcoal (Fe-AC) with a graphene-like structure from biomass waste. The Fe atoms were uniformly dispersed on the activated charcoal support, which possessed a high surface area. This not only significantly increased the number of catalytic active sites but also enhanced electron transfer efficiency, substrate mobility, and collision probability. Compared to pristine activated charcoal, the synthesized Fe-AC exhibited multiple enzyme-mimetic activities, including oxidase-like, peroxidase-like, and catalase-like activities. By leveraging its peroxidase-like activity in conjunction with nitrite-specific diazotization reactions, we developed a portable, smartphone-assisted, on-site ratiometric colorimetric hydrogel sensor for nitrite detection. Utilizing smartphone-based digital imaging, this sensor enabled the quantitative analysis of nitrite at concentrations ranging from 1 to 200 μmol/L, with a detection limit as low as 1 μmol/L. The approximate range of hazardous nitrite concentrations could be easily identified with the naked eye, and the proposed strategy was successfully applied to real sample analysis. This sensor not only maximizes the utilization of waste resources, thereby reducing production costs, but also offers greater economic feasibility and environmental sustainability. Given these advantages, it holds promise for broader applications in various fields.
研究领域:
材料科学
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环境科学
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食品科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yifan Zhang,Sylvestre Ndayiragije,Ming Chen,Xiaobo Wang,Lihua Zhu,Nan Wang
Fe- and nitrogen-doped carbonaceous (Fe-N-C) sites supported on MnO 2 (Fe-N-C@MnO 2 ) were prepared by a solvent-free mechanochemical method for peroxymonosulfate (PMS) activation to degrade norfloxacin (NFX). After a 50-min ball milling of iron(II) phthalocyanine (Fe( II )Pc) and MnO 2 at a weight ratio of 7.5 %, the obtained Fe-N-C@MnO 2 exhibited exceptional activity in PMS activation, achieving nearly complete degradation of NFX in 5 min with a rate constant of 0.62 min −1 . This rate constant was 11.5 and 28.2 times higher than that for milled MnO 2 (bm-MnO 2 ) and the mixture of Fe( II )Pc and MnO 2 , respectively. Alternative iron sources (FeSO 4 , FeCl 2 , Fe(III)-EDTA) and phthalocyanine showed no enhancement. Characterization revealed Fe-N-C@MnO 2 possessed abundant Mn 3+ , oxygen vacancies and Fe-N-C sites. Combined experimental and computational studies demonstrated Fe-N-C@MnO 2 simultaneously enhanced the 1 O 2 generation and facilitated the formation of SO 4 •− , •OH and O 2 •− , with contributions to NFX degradation following: 1 O 2 > •OH ≈ O 2 •− > SO 4 •− . This work establishes mechanochemical coordination engineering as a facile strategy for constructing high-performance metal-N-C hybrid catalysts.
研究领域:
环境科学
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催化
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材料化学
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机械化学
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水处理
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Zhaotian Chen,Juan Wang,Sibudjing Kawi,Qin Zhong
Developing high-efficiency bifunctional electrocatalysts capable of overcoming the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is an urgent challenge for rechargeable zinc-air batteries (RZABs). Herein, we successfully prepared an excellent bifunctional catalysts through facile pyrolysis-free method. Nickel/iron layered double hydroxide (NiFe-LDH) with OER activity was in situ grown on carbon nanotubes (CNTs) and iron (II) phthalocyanine (FePc) with ORR activity was introduced through π-π interaction and covalent functionalization. Furthermore, the intervention of CNTs transform the electronic structure of NiFe-LDH to further enhance OER activity, while solve the problems of poor electrical conductivity and aggregation of FePc. The prepared bifunctional catalyst FePc-LDH@CNTs exhibits preeminent electrocatalystic performance for ORR ( E 1/2 = 0.815 V) as well as OER ( E j=10 = 1.447 V). It displays a prominent bifunctionality which Δ E is only 0.632 V. Moreover, the liquid RZABs based on the FePc-LDH@CNTs demonstrate a significant specific capacity (810.4 mAh g −1 ) and robust stability (840 h), superior to commerical Pt/C + RuO 2 . As flexible RZABs, it maintains superb stability (100 h) and can drive water splitting to produce H 2 smoothly. In addition, the reasons for the failure are dissected by analyzing the components of the battery after cycles. This study provides a novel facile direction to prepare high-efficient and stable bifunctional oxygen electrocatalysts without pyrolysis.
研究领域:
材料科学
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电化学
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储能
·
纳米技术
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yangke Long,Guicong Xiao,Jian Dai,Yanyun Chen,Hua-Yue Zhu,Dan Peng,Huosheng Li
Emerging single-atom materials and metal sulfides hold significant promise as alternatives to precious metal catalysts for nitroaromatics conversion; however, their intrinsic activity and durability remain insufficiently understood. Herein, sulfur and nitrogen co-doped carbon matrices incorporating CoS nanoparticles and single-atom Co with Co–N 4 –S 1 coordination were constructed through a facile pyrolysis approach. Advanced characterization techniques, such as X-ray absorption fine structure (XAFS) and aberration-corrected electron microscopy, unveiled unique structural features underpinning exceptional catalytic efficiency and recyclability. The catalyst achieved a specific catalytic rate of 134 min −1 g −1 L for p -nitrophenol (PNP) hydrogenation, outperforming many noble metal-based catalysts. Experimental and theoretical analyses identified the Co–N 4 –S 1 single-atom moiety as the primary active site, demonstrating remarkable structural stability. Axial sulfur coordination was found to fine-tune the electronic state of the central Co atom, mitigating the overbinding of reaction intermediates and enhancing PNP conversion efficiency. In contrast, CoS nanoparticles exhibited limited recyclability, with agglomeration, cobalt hydroxide formation, and dissolution observed during repeated use. This study presents a highly efficient catalyst for nitroaromatics conversion and provides a foundational framework for understanding the durability and mechanistic roles of cobalt-based active sites.
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
Science Advances
·
2024
·Vol. 10
·期 40
·
IF 11.7
Zhongliang Huang,Yingru Wang,Jing Xia,Shengnan Hu,Nanjun Chen,Tianyi Ding,Changhong Zhan,Chih-Wen Pao,Zhiwei Hu,Wei-Hsiang Huang,Tong Shi,Xiangmin Meng,Yong Xu,Liang Cao,Xiaoqing Huang
Pt-based nanoparticles (NPs) have been widely used in catalysis. However, this suffers from aggregation and/or sintering at working conditions. We demonstrate a robust strategy for stabilizing PtCo NPs under high temperature with strong interaction between M–N–C and PtCo NPs with Pt–M–N coordination, namely, “atom glue.” Such atom glue for stabilizing Pt-based NPs can be extended to Zn, Mn, Fe, Ni, Co, and Cu, being a versatile strategy for stabilizing PtCo NPs, which substantially promotes the performance toward oxygen reduction reaction (ORR) and fuel cell. Impressively, the mass activity (MA) reaches 2.99 A mgPt−1 for ORR over g-Zn–N–C/PtCo, and 79.3% of the initial MA is maintained after 90K cycles in fuel cell. This work provides a versatile strategy for stabilizing Pt-based NPs via atom glue, which is likely to spark widespread interest across various fields.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science China-Chemistry
·
2025
·
IF 9.7
Liu Jie,Ye Qiu,Wu Yi,Chen Junliang,Ge Yongjie,Zhang Linjie,Abazari Reza,Qian Jinjie
Molecular catalysts like metal phthalocyanines (MPc) hold significant promise for diverse applications in renewable energy conversion and storage. Despite their inherent catalytic activity in the oxygen reduction reaction (ORR), enhancing their practical applicability necessitates addressing challenges in electrical conductivity and catalytic stability through effective control of electron distribution within the substrate. In this work, we have successfully synthesized an electrocatalyst featuring FePc molecules anchored onto N,S co-doped carbon nanorods from a pillar-layer metal-organic framework (MOF), designated as ZTB-NSCR-FePc. This MOF-derived heteroatom-doped carbon substrate could be easily obtained by direct pyrolysis of a pre-fabricated rod-like Zn-TDC-bpy. The optimized ZTB-NSCR-FePc demonstrated exceptional electrocatalytic efficiency and stability towards ORR with a positive half-wave potential of 0.890 V. When employed in a Zn-air battery, it outperformed the benchmark Pt/C air cathode, achieving a peak power density of 198.9 mW cm −2 . Finally, theoretical calculations revealed that short-range electron interactions between N/S atoms and the graphene substrate significantly enhance the anchoring effect of FePc, improve the adsorption of reaction intermediates, and thereby boost the ORR performance.
研究领域:
材料科学
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电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）