CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xiao Zhang,Zhongping Yao,Yang Zhou,Zhirong Zhang,Guifeng Lu,Zhaohua Jiang
The construction of dual electron reaction centers is an attractive strategy to accelerate the rate-limiting step in Fenton-like catalyst. In this work, we constructed the dual electron reaction centers and electron transport path over C–O–Fe bridges connected by graphene oxide (GO) and Fe 3 O 4 through density functional theory (DFT). The calculations show that there is a strong interaction of C–O–Fe between GO and Fe 3 O 4 , and electrons around C would transfer to Fe along C–O–Fe linkages and the electron-rich reaction microcenters are generated around Fe. Based on it, Fenton-like catalyst of ultra-small Fe 3 O 4 (less than 10 nm) loaded on 3D reduced graphene oxide (rGO) (composite denoted as rGF) was successfully prepared. Characterization analyses have demonstrated that C–O–Fe bonds exist in rGF and CV test confirmed the cross-linked structure implemented by C–O–Fe is thermodynamically beneficial for electrons transport to Fe which is responsible for the regeneration of Fe(II). When the weight ratios of GO to Fe 3 O 4 reach 5%, rGF-5, the optimized composite displays superior Fenton-like performance that the removal efficiencies of tetracycline hydrochloride (TCH) are 98.7% within 60 min and 96.1% within 90 min, with the initial pH 4.5 and pH 6.7, respectively. The excellent cyclic stability of rGF-5 further verifies the structure of electron-rich reaction microcenters on C–O–Fe bond bridges is well established to ensure that Fenton-like reactions continue to occur efficiently. The results of mass spectrometry indicate that products with m / z = 114 converted from TCH ( m / z = 445) accounted for 87% at 60 min. This work not only achieves a way to construct high-performance heterogeneous Fenton-like catalysts for degradation of antibiotics, but also provides a new insight for designing various efficient catalysts based on the theoretical guidance.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2020
·Vol. 22
·期 20
·11508-11518
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IF 3.43
Jing Chen,Hanling Yang,Hongquan Fu,Hongyan He,Qiang Zeng,Xuehui Li
Electrochemical oxidation is a promising and effective method for lignin depolymerization owing to its selective oxidation capacity and environmental friendliness. Herein, the electrooxidation of non-phenolic alkyl aryl ether monomers and β-O-4 dimers was experimentally (by cyclic voltammetry, in situ spectroelectrochemistry, and gas chromatography-mass spectroscopy) and theoretically (by DFT calculations) explored in detail. Compared to the reported literature (T. Shiraishi, T. Takano, H. Kamitakahara and F. Nakatsubo, Holzforschung, 2012, 66(3), 303–309), 1-(4-ethoxyphenyl)ethanol showed a distinguishable oxidation pathway, where the resulting carbonyl product surprisingly underwent a bond cleavage on alkyl–aryl ether to ultimately produce a quinoid like compound. In contrast, β-O-4 dimers, like 2-phenoxy-1-phenethanol and 2-phenoxyacetophenone also demonstrated electrochemical oxidation induced by Cβ–O and Cα–Cβ bond cleavages. For the oxidation products, the presence of the Cα-hydroxyl group in dimers was the key to selectively generate aldehyde-containing species under mild electrochemical conditions, otherwise it produces alcohol-containing products following a different mechanism compared to the CαO containing dimers.
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PubMed
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
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IF 3.8
Chuhan Zhang,Yanchang Chu,Linying Fu,Qiuyue Wang,Rui Ma,Donghai Xu,Le Yang
Lignin, a renewable resource rich in aromatic ring structures in nature, is an ideal natural source to produce aromatic compounds and cycloparaffin. Herein, we prepare MOF-derived Ni–MoxC/C and Co–MoxC/C as catalysts for the depolymerization of lignin and dimeric model compounds. Diphenyl ether (DPE) with 4-O-5 bond, benzyl phenyl ether (BPE) with α-O-4, and phenethyl phenyl ether (PPE) with β-O-4 are chosen as dimeric model compounds. Overall, Ni–MoxC/C and Co–MoxC/C show distinguished different activity toward product distribution. Ni–MoxC/C facilitates both C–O bond cleavage and hydrogenation of the benzene ring, and the main products are ethyl cyclohexane and cyclohexanol for all three model compounds. In contrast, Co–MoxC/C only facilitates C–O bond cleavage and obtains phenol and ethylbenzene as products. Similarly, for the depolymerization of lignin, cycloparaffins are obtained on Ni–MoxC/C, while phenol, guaiacol, 2,6-dimethoxyphenol, and their respective derivatives are obtained on Co–MoxC/C.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuyan Feng,Dongbo Wang,Qingge Feng,Chenghua Fan,Ying Lu,Wenqiang Yang
Activation of peroxymonosulfate (PMS) to generate reactive oxygen species (ROS) for pollutant degradation via metal-free photocatalysts is an important green wastewater treatment and remediation method, but the pathway for generating ROS via exciton effects in catalysts is often overlooked. In this study, OH/C=O co-modified N-defective rod-shaped carbon nitride (Nv-CN-O) was designed and synthesized by soft template and alkali hydrothermal method. In the Nv-CN-O/PMS/Light system, there was a synergistic degradation of tetracycline (TC) by carriers and excitons, with a degradation rate 2.15 times higher than that of CN/PMS/Light. N vacancies and OH/C=O enhanced the adsorption to PMS, accelerated the charge transfer process, and activated PMS to generate ·O 2 − dominated reactive species. The functional group OH/C=O promoted the production of triplet excitons that through the energy transfer pathway to promote the production of 1 O 2 . Abundant ROS were involved in the TC degradation process, and three possible TC degradation pathways were proposed. Nv-CN-O has strong anti-interference ability in actual water bodies, shows a promoting effect on the degradation of TC, which has practical application potential.
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FUEL
·
2020
·
IF 5.578
Tianjin Li,Hongfei Lin,Xinping Ouyang,Xueqing Qiu,Zechen Wan,Tao Ruan
The selective cleavage of C–O bond in lignin is the key to convert them into aromatic compounds and then to produce liquid fuels and chemicals. N-doped carbon nanosheets were obtained by direct pyrolysis of glucosamine hydrochloride (GAH) and melamine. Highly-dispersed and small-sized Ru nanoparticles (NPs) supported N-doped carbon by impregnation method, which can efficiently convert lignin to obtain 40.70% aromatic monomers. It was 2.3 times than that of the commercial catalyst (Ru/C) and the catalyst could be used at least five runs with an insignificant loss in the yield of aromatic monomers. The morphology, specific surface area, nitrogen species and content of supports could be tuned by controlling the weight of melamine. The results showed that the melamine and GAH were condensed to form layered graphitic carbon nitride (g-C 3 N 4 ) and a carbon skeleton at 600 °C, respectively. Then, the produced N from the decomposition of g-C 3 N 4 at high temperature (>700 °C) could improve nitrogen concentration, increase the specific area and result in the graphene-like wrinkled morphology. The presence of pyridinic N not only served as metal coordination sites to stabilize and disperse Ru NPs but also enhanced the proportions of Ru 0 through the electronic interactions. The DFT calculations implied that the pyridinic N contributed to the highest adsorption energy for 2-phenoxy-1-phenethanol (PPE) and a reduction of the disassociation energy for C alkyl –O bond compared with graphite N and pure C.
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POLYMER DEGRADATION AND STABILITY
·
2020
·
IF 4.032
Hongyan Li,Xianglin Hou,Lin Chai,Xiaojing Cui,Yingxiong Wang,Tiansheng Deng
The degradation and recovery of waste rigid polyurethane foam (RPUF) have confronted enormous challenge because of its three-dimensional network. An efficient strategy was developed for chemical recycling of high value-added aromatic polyamines and polyether polyols via selective cleavage of carbamate and urea bonds from RPUF and characterized by Nuclear Magnetic Resonance (NMR) and Fourier Transform Infrared Ray (FT-IR). The carbamate and urea bonds were readily cleaved using (NH 2 ) 2 CO/CH 3 CH 2 OH as degradation system at 180 °C for 10 h. Nevertheless, the C–C bonds and C–O–C of ether linkages as framework structure remained intact in the degradation process. Eventually, the high value-added products including aromatic polyamines and polyether polyols were retrieved. A feasible mechanism for degradation was proposed based on the NMR observations.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yehan Xiong,Bingchang Chen,Tiantian Xu,Yu Zhou,Pengcheng Gao,Jianguo Bao
Current research has found that C=O groups hold a significant position in the oxidation process of peroxymonosulfate (PMS) in the activated carbon system, influencing both the generation of reactive species and the degradation of organic contaminants. Quinone organic compounds, which are rich in C=O groups, exhibit high reactivity but also inherent toxicity. Additionally, these compounds decompose easily at high temperatures, complicating their use in carbon-based materials. This study introduces a novel approach to enhance the content of C=O groups in carbon materials by controlling the synthesis of sulfur heterocyclic organic quinone (SHQ) precursors. For the first time, we established a sulfur heterocyclic organic quinone-derived carbon (SHQC)/PMS system, where SHQC catalysts demonstrate remarkable catalytic efficiency in activating PMS for the degradation of organic pollutants. In different natural water matrices, the removal rate of tetracycline hydrochloride (TC) exceeds 90 % under optimized conditions (SHQC-9: 0.2 g L −1 , PMS: 1 mM, TC: 4.45 mg L −1 ). The C=O group was identified as the active site for PMS activation through a combination of quantitative structure-activity relationships, specific site blocking, and antithesis methods. The activation mechanism was elucidated through scavenger experiments and electron paramagnetic resonance (EPR) analysis. The results indicate that the superior catalytic performance of the SHQC-9/PMS system is due to a non-radical pathway, with singlet oxygen ( 1 O 2 ) being the primary species responsible for TC degradation. These findings offer a novel pathway for designing highly efficient, safe, and environmentally friendly carbon material catalysts.
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PubMed
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Qianqian Zhang,Yaru Zhu,Min Yang,Yanru Zhang,Jialin Wang,Shanshan Liu,Ye Liu,Xin Yang,Kai Feng,Wenzuo Li
Aqueous zinc-ion batteries (AZIBs) have good application prospects in the field of large-scale energy storage. The design and synthesis of high-performance cathode materials are key to promoting the development and application of AZIBs. In this work, the combination of redox active V 4+ cation and HPO 3 2− anion provides excellent zinc-ion (de)intercalation ability. In addition, HPO 3 2− and C 2 O 4 2− anion groups collaborate to construct a stable framework with multi-dimensional zinc-ion transport channels, providing fast and robust pathway for zinc-ion transport. Carbon composites further improve electronic conductivity, shorten ion transport distance, and increase the electrochemical reaction area of Na 2 [(VO) 2 (HPO 3 ) 2 (C 2 O 4 )]·2H 2 O@C (NVPCO@C) cathode material. As a result, NVPCO@C cathode material delivers a high specific capacity over 180 mAh·g −1 at a current density of 40 mA·g −1 . Moreover, NVPCO@30%C cathode material maintains 100 % capacity after 100 cycles. Ex-situ X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Raman spectra confirm the electrochemical activity of V 4+ /HPO 3 2− ions and reveal the zinc-ion storage mechanism.
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高影响因子
TETRAHEDRON
·
2014
·
IF 2.817
Dazhuang Miao,Xuesong Shi,Guozhen He,Yao Tong,Zengqiang Jiang,Shiqing Han
N -(2-Chloro-phenyl)-2-halo-benzamides (halo=I/Br/Cl) as substrates were used for the one-pot synthesis of 2-arylbenzoxazole derivatives via copper-catalyzed intermolecular C–N/intramolecular C–O couplings with primary amines . This aryl amination offers clean reaction conditions and easy work-up in good yields by using CuI as catalyst, readily available 8-hydroxyquinoline as ligand, K 3 PO 4 as base, DMF as solvent.
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高影响因子
JOURNAL OF POWER SOURCES
·
2026
·
IF 8.4
Guanghui Zhou,Yumeng Jia,Kai Chen,Haiguang Gao,Jian Zang,Yucheng Huang,Juan Xu,Jianyu Cao
Organic cathode materials present a highly viable alternative, offering abundant resources, environmental compatibility, and highly designable molecular structures. However, conventional organic materials suffer from high solubility and low electronic conductivity. To overcome these inherent drawbacks, we propose a structural design strategy based on constructing extended π-conjugated molecular frameworks with high-density electrochemically reversible groups. Inspired by this strategy, we synthesized a novel sulfur-linked C3-symmetric conjugated organic compound, tris-benzothioxanthenedione 2,3-b (denoted as 6S6O), via a facile condensation reaction. The unique structure of 6S6O provides multiple high-density C=O/C=N moieties for reversible lithium storage, excellent solvent tolerance, and high intrinsic conductivity due to electron delocalization. Electrochemical testing demonstrates outstanding performance in a Li//6S6O half-cell, delivering a high reversible capacity of 352 mAh g −1 at 0.1 A g −1 , corresponding to a high energy density of ∼748.6 Wh kg −1 . Importantly, the electrode demonstrates excellent rate capability (retaining 65.3% capacity with a 20-fold current increase) and superior long-term cycling stability, maintaining 77.5% capacity retention over 2409 cycles at 2 A g −1 . Ex situ characterization and DFT calculations confirm a highly reversible, capacitive-controlled Li + storage mechanism involving the C=O and C=N bonds of the quinone/pyrazine units. The results validate the effectiveness of the extended π-conjugated design for developing high-performance organic cathode materials.
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高影响因子
ENERGY
·
2025
·
IF 9.4
Yulei Zhang,Zonglu Yao,Junyi Ma,Jiadong Yu,Ping Ai,Ruixia Shen,Yi Liang,Lixin Zhao
Low interspecies electron transfer efficiency among microorganisms is a critical factor limiting anaerobic digestion performance. In this study, conductive and stable biochar (BC) was combined with redox-active anthraquinone-2-sulfonate (AQS) to enhance electron transfer efficiency through their synergistic effects, thereby improving the efficiency of anaerobic digestion. Results showed that cumulative methane production (CMP) reached 176.34 mL/g VS under optimal conditions, including an AQS impregnation concentration of 1 mmol/L, a BC/AQS addition of 5 %, and a total solid (TS) content of 10 %. The addition of BC/AQS enriched Proteiniphilum and Methanobacterium , which shifted the methanogenic pathway from acetoclastic to hydrogenotrophic, significantly improving volatile fatty acid conversion and total organic carbon degradation. Redundancy analysis (RDA) and changes in key enzyme-encoding genes indicated that BC/AQS enhances the synergistic interaction between Proteiniphilum and Methanobacterium through the redox activity of quinone/C=O functional groups, which may play a key role in the formation of direct interspecies electron transfer (DIET). This study provides a promising strategy to enhance microbial electron transfer mechanisms in anaerobic digestion by leveraging the complementary properties of meso-materials, offering new insights into the utilization of agricultural waste for energy production.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Han-Bing Gao,Yue-Lun Wang,Dao-Ran Liu,Jin-Xuan Xie,Le-Le Qiu,Jian Xiao,Jing Liang,Fang-Jing Liu,Yun-Peng Zhao
Achieving high efficiency and selectivity in cleaving aryl C–O bonds is critical for lignin valorization and the production of aromatic chemicals. A green and sustainable approach has been developed using bimetallic Ni–W catalysts, which controlled the hydrogen supply and mediated hydrogen transfer via in situ hydrogen donors. An appropriate W/Ni ratio is essential for enhancing the supply of active hydrogen, the adsorption capacity for reactive molecules, and the efficiency of hydrogen transfer, thereby optimizing the overall catalytic performance. A comprehensive investigation was conducted on the factors influencing the catalytic transfer hydrogenolysis of lignin derivatives, focusing on the reaction temperature, solvent, hydrogen source, pressure, and duration. Under optimal conditions (180 °C, 1.0 MPa N2, and <2.5 h), various lignin-derived aryl ethers achieved complete conversion with 100% monomer selectivity. This study demonstrated the excellent reusability of the Ni–W catalyst for four cycles. More significantly, the mechanisms underlying active hydrogen transfer, transfer hydrogenolysis, and bimetallic interactions were elucidated. The integration of Ni and W species significantly enhanced the synergy among active metal sites, oxygen defects, and acid sites. This synergistic mechanism enabled H• and H+ to function as the primary active hydrogen species. Furthermore, the in situ generation and targeted migration of H• radicals and H+ ions facilitated the preferential cleavage of C–O bonds over the hydrogenation of aromatic units within lignin, leading to the formation of high-value aromatic monomers.
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