Journal of Energy Chemistry
·
2024
·
IF 14
Yingzheng Li,Shaoqi Zhan,Zijian Deng,Meng Chen,Yilong Zhao,Chang Liu,Ziqi Zhao,Hongxia Ning,Wenlong Li,Fei Li,Licheng Sun,Fusheng Li
Inspired by the function of crucial components in photosystem II (PSII), electrochemical and dye-sensitized photoelectrochemical (DSPEC) water oxidation devices were constructed by the self-assembly of well-designed amphipathic Ru(bda)-based catalysts (bda = 2,2ʹ-bipyrdine-6,6ʹ-dicarbonoxyl acid) and aliphatic chain decorated electrode surfaces, forming lipid bilayer membrane (LBM)-like structures. The Ru(bda) catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O–O formation mechanisms. However, compared to the slow charge transfer process, the O–O formation pathways did not determine the PEC water oxidation efficiency of the dye-sensitized photoanodes, and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs. Instead, charge transfer plays a decisive role in the PEC water oxidation rate. When an indolo[3,2-b] carbazole derivative was introduced between the Ru(bda) catalysts and aliphatic chain-modified photosensitizer in LBM films, serving as a charge transfer mediator for the tyrosine-histidine pair in PSII, the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Moxing Cheng,Haoyun Sheng,Yin’an Zhu,Ziqi Tian,Yichao Lin
The development of highly active and durable catalysts for the acidic oxygen evolution reaction (OER) is urgently needed to accelerate reaction kinetics and reduce energy barriers. Herein, we propose to tune the local electronic structure in RuO 2 via yttrium ion (Y 3+ ) doping to facilitate the OER process following oxide path mechanism (OPM). The electron-deficient of Y 3+ redistributes local charge density, strengthens metal–oxygen bonds to suppress lattice degradation. Moreover, the incorporation of larger Y 3+ radius reduce the Ru–Ru distance, and thereby benefits O–O coupling. The optimized Y 0.11 Ru 0.89 O 2−δ catalyst exhibits an exceptionally low overpotential of 195 mV at 10 mA cm −2 for acidic OER and operates stably for 250 h at 100 mA cm −2 in a PEM electrolyzer. Theoretical investigations reveal that Y–O–Ru structure effectively modifies the chemical environment and optimizes the atomic configuration of active sites. This study establishes electron-deficient, large-radius dopants as an effective strategy for designing efficient and durable acidic OER catalysts, enhancing RuO 2 performance.
研究领域:
电催化
·
材料化学
·
能源科学
·
表面科学
·
无机化学
·
电化学工程
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Ping Xin,Hongjiang Li,Ziwei Huang,Kexin Su,Ying-Ying Gu
To address the challenges of low selectivity and poor stability in hydrogen peroxide (H 2 O 2 ) electrosynthesis within neutral media, this study developed an O/N co -doped carbon nanotube-polytetrafluoroethylene composite cathode (designated as GF/ONCNTs-6/PTFE). Through precise control of the synergistic effects between pyrrolic-N doping (40.7 %) and carboxyl/ether functional groups, the adsorption of *OOH intermediates was significantly enhanced; simultaneously, PTFE micro-cracks were employed to establish triple-phase interfaces for facilitated oxygen diffusion. The cathode achieved a high H₂O₂ yield of 139.45 mg/L under neutral conditions (pH 7), with a current efficiency of 67.06 %, and exhibited only 8.2 % activity loss after 10 cycles. In an integrated electro-Fenton system, it accomplished 98.8 % degradation of methyl orange within 2 h under optimal conditions. This work demonstrates that defect engineering and O/N functionalization in composite cathodes significantly boost 2e − ORR efficiency, offering a promising laboratory-scale platform for electrochemical wastewater purification
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ACS Macro Letters
·
2026
·
IF 4.9
Shu Nian-Zu,Li Hao-Tian,Peng Yu-Qing,He Guo-Long,Gu Jie,Li Yong-Qing,Cao Yu-Cai,Zhang Chuan-Lei
The synthesis of ultrahigh-molecular-weight polyethylene
(UHMWPE)
is often hampered by the inherent compromise in traditional catalysts,
such as Ziegler–Natta systems, which struggle to balance high
activity with precise control over molecular parameters. Covalent
organic frameworks (COFs) offer a promising alternative, allowing
for atomic-level design through their tunable pores and microenvironments.
In this work, we address this challenge by designing a series of Zr@COF
catalysts─denoted as Zr@PQ-TFPB (O–Zr–O), Zr@PQSO-TFPB
(N–Zr–O), and Zr@PQDO-TFPB (N–Zr–N)─to
systematically investigate the role of the coordination environment.
Spectroscopic and catalytic studies reveal that the N–Zr–N
configuration in Zr@PQDO-TFPB optimally reduces the electron density
at the Zr center. This electronic modulation, characterized by reduced
electron density at the Zr center, facilitates ethylene adsorption/insertion
while suppressing β-H elimination, leading to a superior polymerization
activity of 3.87 × 10 5 g·mol Zr –1 ·h –1 at 3.0 MPa─66%
and 38% higher than its O–Zr–O and N–Zr–O
analogues, respectively. This catalyst produces UHMWPE with a high
molecular weight of 1.71 × 10 6 g·mol –1 and a relatively narrow dispersity ( Đ = 2.2).
Furthermore, the rigid nanochannels of the COF provide a confining
effect that stabilizes the growing polyethylene chains. Our findings
underscore a critical synergy between coordination-induced electronic
effects and spatial nanoconfinement, providing a novel design principle
for next-generation polyolefin catalysts.
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高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Zong-Pin Fu,Qi-Jie Zhou,Yun-Peng Zhao,Yu-Fa Wu,Fang-Jing Liu,Mei Zhong,Jian Li,Jing Liang,Jing-Pei Cao
The abundant bridging bonds and side chains in lignin make the selective cleavage of its C-O bonds a promising approach for achieving efficient conversion. Herein, Cu/CoOx-CeO 2 catalysts were prepared and the effects of their physical and chemical structures on C-O bond hydrogenolysis activity were investigated. The results indicated that incorporating an appropriate amount of CeO 2 as a support facilitated the doping of Co n+ cations into the CeO 2 lattice, enhancing oxygen vacancy concentration. Additionally, the Cu K-edge X-ray absorption near-edge structure (XANES) spectra revealed that Cu exists in a mixed valence state (Cu δ+ , 0 < δ < 2) within the catalyst. Reaction pathway regulation was achieved through strategic modulation of reaction conditions. When isopropanol was used as the solvent under a N 2 atmosphere, 2-phenoxy-1-phenylethanol (2-PPE-ol) was completely converted at 180 °C within 2 h, yielding ethylbenzene and cyclohexanol with 100 % selectivity. Conversely, when n -hexane was employed as the solvent, dehydrogenation of the C α -OH group generated hydrogen radicals, which promoted cleavage of the C β -O bond in the β-O-4 ketone intermediate, resulting in phenol and 1-phenylethanol with 100 % selectivity. Isotopic labeling and active hydrogen tracking experiments revealed that the active hydrogen in catalyst transfer hydrogenolysis (CTH) originated from the solvent, whereas self-hydrogen-transfer hydrogenolysis (SHTH) relied on hydrogen derived from the C α -OH group of 2-PPE-ol. This work provides valuable insights into the directional conversion of lignin into high-value chemicals and efficient energy utilization.
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LANGMUIR
·
2020
·
IF 3.557
Wenting Kong,Yunlu Pan,Bharat Bhushan,Xuezeng Zhao
The separation of oil–water emulsion using superliquiphobic/philic porous coated materials has attracted considerable attention for dealing with environmental pollution and resource recycling issues. The coatings used may lack adequate surface mechanical and chemical durability. This paper proposes a simple method without other modifications for separating the oil–water emulsion. A porous layer was fabricated by superhydrophilic Al2O3 particles, which could separate oil–water emulsions. The particle layer has the property of underwater superoleophobicity after prewetting. For the oil-in-water (O/W) emulsion separation, a 0.3 μm Al2O3 particle layer was used. This layer had a pore size less than about 1 μm to minimize oil flow and to obtain a purity of oil recovery greater than 99 wt %. For the water-in-oil (W/O) emulsion separation, a 40 μm Al2O3 superhydrophilic particle layer was used. Larger particles were used to provide a more porous surface to facilitate oil flow through the layer, resulting in a purity of water recovery purity greater than 99 wt %.
研究领域:
环境科学
·
材料科学
·
分离技术
·
表面化学
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
·
IF 3.99
Jing Guo,Jianguo Jiang,Xiaolong Gu,Xia Li,Tianqing Liu
Multiple emulsions provide a facile route for particle preparation due to their ability to be used as liquid templates. Herein, biocompatible oil-in-water-in-oil (O 1 /W/O 2 ) double emulsions were fabricated using a two-step procedure and applied as templates for preparation of calcium alginate hydrogels with encapsulated β-carotene. The encapsulation efficiency ( EE ) of β-carotene showed a positive correlation to the outer-to-inner droplet size ratio of the O 1 /W/O 2 emulsion. The maximum EE , ∼50 wt%, could be achieved in the freshly prepared O 1 /W/O 2 emulsion when using aqueous alginate of 2 wt% as the intermediate phase and β-carotene-loaded R-(+)-limonene of 0.1 wt% as the inner oil phase. Gelation of the alginate phase was induced by addition of a small amount of aqueous CaCl 2 into the β-carotene-loaded O 1 /W/O 2 emulsion. The resulting hydrogels in water were characterized by laser diffraction and several microscopy measurements. The hydrogels showed good spherical shape and their average size was a little larger than that of the emulsion droplet templates. This work contributed to the understanding of encapsulation in O 1 /W/O 2 emulsion system and provided a novel methodology for encapsulation of carotenoids and other lipophilic bioactives.
研究领域:
食品科学
·
材料科学
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高影响因子
CHINESE CHEMICAL LETTERS
·
2013
·Vol. 24
·期 12
·1091-1094
·
IF 1.21
Xin-Ping Ouyang,Chun-Lei Liu,Yu-Xia Pang,Xue-Qing Qiu
A trimeric lignin model compound composed of α - O -4 and β - O -4 linkages was prepared by the microwave-assisted synthesis, which consisted of three steps: (a) the synthesis of 3-methoxy-4-benzyloxyacetophenone ( 2 ) from acetovanillone ( 1 ), (b) the bromination of compound 2 to produce 3-methoxy-4-benzyloxy- α -bromoacetophenone ( 3 ), and (c) followed by a nucleophilic substitution of compound ( 3 ) to obtain 3-methoxy-4-benzyloxy- α -(3-methoxy-4-(1-propenyl)phenol)-acetophenone ( 4 ). The target product was characterized by MS, 1 H NMR and 13 C NMR spectroscopy. It was found that the trimeric compound synthesized can be used as a preferable lignin model compound because it contains guaiacyl structural unit (3-methoxy-4-hydroxy phenyl propane) linked by α - O -4 and β - O -4 linkages. In addition, under the conditions of microwave irradiation, the reaction time of each step is significantly reduced, and the selectivity of target product is greatly improved. The yields of each step and the overall sequence are 95.31%, 87.3%, 90.6% and 75.4% (95.31% × 87.3% × 90.6%), respectively.
研究领域:
有机化学
·
高分子化学
·
绿色化学
·
生物质转化
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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 .
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2022
·
IF 12.545
Ruirui Shi,Wenting Zou,Zhiling Zhao,Guanqun Wang,Min Guo,Shiyun Ai,Qing Zhou,Fengchun Zhao,Zhengyou Yang
In this work, a green, harmless and signal-amplified electrochemical immunosensor based on phage-mimotope M31 (C–P-D-G-N-H-V-P-F-C) and horseradish peroxidase (HRP) was constructed for detecting O,O -dimethyl organophosphorus pesticides (OPs). The glassy carbon electrode (GCE) was modified by nitrogen and boron doped carbon quantum dots and graphene oxide (NBCQDs@GO) which can provide sufficient surface area and enhance the conductivity of the electrode. The O,O -dimethyl OPs class specific antibody mAb3C9 was assembled onto the NBCQDs@GO and the phage-mimotope M31 competitively bound to mAb3C9 with OPs. Furthermore, large amounts of anti-M13 mAb-HRP were introduced to the electrode through thousands of binding sites on the capsid of phage. HRP can catalyze 4-chloro-1-naphthol (4-CN) to produce insoluble precipitates (Benzo-4-chlorhexanedione, 4-CD). Hence, the concentration of OPs can be quantified by measuring impedance signal with electrochemical impedance spectrum (EIS). Under the optimal detection conditions, the 50% inhibitory concentration (IC 50 ) and limits of detection (LODs) values of 9 O,O -dimethyl OPs were in range of 0.989–4.017 ng/mL and 0.003–0.014 ng/mL, respectively. The recovery rates of spiked OPs in cucumber, cabbage and lettuce were 88.20–112.50% with coefficient of variation from 2.97 to 15.64%. Therefore, the immunosensor showed very good sensitivity and demonstrating potential application for the detection of O,O -dimethyl OPs in food samples.
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高影响因子
Nanomaterials
·
2019
·Vol. 9
·期 2
·E210
·
IF 4.034
Qingtong Zhang,Mingfu Li,Chenyan Guo,Zhuan Jia,Guangcong Wan,Shuangfei Wang,Douyong Min
Lignin is the second largest naturally renewable resource and is primarily a by-product of the pulp and paper industry; however, its inefficient use presents a challenge. In this work, Fe₃O₄ nanoparticles loaded on lignin nanoparticles (Fe₃O₄@LNPs) were prepared by the self-assembly method and it possessed an enhanced peroxidase-like activity. Fe₃O₄@LNPs catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of H₂O₂ to generate a blue color, was observable by the naked eye. Under the optimal conditions, Fe₃O₄@LNPs showed the ability of sensitive colorimetric detection of H₂O₂within a range of 5⁻100 μM and the limit of detection was 2 μM. The high catalytic activity of Fe₃O₄@LNPs allows its prospective use in a wide variety of applications, including clinical diagnosis, food safety, and environmental monitoring.
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高影响因子
ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Kedir Ebrahim Ahmed,Dong-Hau Kuo,Worku Lakew Kebede
Heterojunction construction with low band gap materials is an effective way of utilizing UV light active materials under visible light irradiation. Here, we report the synthesis of Bi 2 (O,S) 3 /Zn(O,S) heterostructure using simple solvothermal method without surfactant. The catalysts were investigated with different characterization techniques. All the composite catalysts showed high light absorption capacity in the whole visible light spectrum. The catalytic activity of the catalysts was evaluated by Cr(VI) reduction. While pure Zn(O,S) catalyst showed no significant Cr(VI) reduction, higher photocatalytic activity than individual components were exhibited after heterojunction construction with Bi 2 (O,S) 3 . 20-BiZnOS catalyst with Bi/Zn molar percentage of 20% showed the best photocatalytic activity among the composites with 99.5% Cr(VI) reduction within 12 min under visible light irradiation. Heterojunction formation between Bi 2 (O,S) 3 and Zn(O,S) nanoparticle, and selective adsorption of Cr(VI) and desorption of Cr(III) on the surface of 20-BiZnOS composite catalyst were ascribed to the enhanced photocatalytic activity of the composite catalyst.
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危险品化学品经营许可证（带存储）