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.
研究领域:
环境科学
·
催化化学
·
废水处理
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2020
·
IF 4.089
H. Liu,X. Yang,S. Cao,F. Yu,S. Long,J. Chen,M. Zhang,S. Parkin,T. Li,Z. Yang
A series of N-phenyl-2-hydroxynicotinanilides (PHNAs) have been synthesized, and their crystal structures have been investigated. The identity of these compounds is revealed to be the tautomer of PHNAs, i.e., 2-oxo-1,2-dihydropyridine-3-carboxylic acid phenylamides, compounds with both amide and lactam functionalities. Among these compounds, those with no or negligible steric hindrance take a near planar conformation and form lactam–lactam dimers, not the widely observed amide NH···O═C hydrogen bond chains, while those with steric hindrance take a twisted conformation and form an amide NH···O═C (lactam) hydrogen bond. A succinct theoretic study combining conformational analysis and molecular electrostatic potential surfaces (MEPS) survey provided a reasonable explanation of the formation of these two different hydrogen bond motifs.
研究领域:
化学
·
晶体学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
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.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Jiajin Zhong,Na Li,Xiaoxuan Xu,Limin Wei,Huijian Liu,Huijuan Li,Zheng Fang,Haifeng Bao
High temperature thermally stable fiber materials with flexibility are expected to be applicable to severe conditions. In this article, ZrO 2 /Si–C–O ceramic fibers have been synthesized by the sol-gel process combined with the electrospinning technique. We focus on the changes of composition, structure and morphology with the increasing heat treatment temperature. More importantly, the effects of ZrO 2 crystalline phase transformation on mechanical property of ZrO 2 /Si–C–O ceramic fibers have been investigated. The results show that the increased temperature can lead to an increase of the fiber diameter and grain size, as well as the transformation of ZrO 2 phase. It is also found that the ZrO 2 /Si–C–O ceramic fibers possess refined crystalline grain and improved mechanical properties at a heat treatment temperature of 800 °C, which is mainly due to the fact that the amorphous Si–C–O phase containing free carbon facilitates the refinement of the crystalline grain, and the ZrO 2 in the tetragonal structure improves the flexibility of ceramic fibers. Furthermore, the obtained fibers exhibit excellent thermal stability up to 1300 °C, therefore they have broad application prospect in high temperature environment.
研究领域:
材料科学
·
陶瓷材料
·
复合材料
·
热工程
✓ 已验证
产品关联
DOI
高影响因子
ORGANOMETALLICS
·
2020
·
IF 3.804
Liangwei Zhang,Long Liu,Tianzeng Huang,Qizhi Dong,Tieqiao Chen
A palladium-catalyzed cyclobutanation of aryl sulfonates with strained alkenes has been developed. The methodology is featured to achieve the cleavage of both C–O and C–H bonds of phenol derivatives in one pot. Under the reaction conditions, in addition to reactive triflates, the relatively inactive tosylates and mesylates can also be transformed into the corresponding benzocyclobutanes in high yields. This reaction can be carried out in gram-scale experiments with a low loading of the palladium catalyst and is applicable to the cyclobutanative modification of bioactive molecules, highlighting its synthetic value in organic synthesis.
研究领域:
有机化学
·
催化化学
·
合成化学
✓ 已验证
DOI
高影响因子
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.
研究领域:
催化化学
·
可再生资源转化
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2022
·Vol. 46
·期 11
·15174-15181
·
IF 4.672
Yang Liu,Xuesong Cai,Dinggui Chen,Yan Qin,Yuan Chen,Jinxiang Chen,Chenglu Liang
Summary The large-scale applications of energy storage system via lithium-ion batteries (LIBs) put forward demands for high capacity, high safety, and low cost of materials. Covalent organic polymers have attracted extensive attention because of their high capacity, flexible structural design, high safety, abundance, and low cost. Here, 2,3,5,6-tetraamino-p-benzoquinone and hexaketocyclohexane octahydrate were chosen as monomers to construct the covalent organic framework (TH-COF) cathode materials with active C=O and C=N groups. The TH-COF was further composed with reduced graphene oxide (rGO) and the prepared TH-COF/rGO cathode provided a capacity of 135 mAh g −1 after 600 cycles at 1 C current density. In addition, after 100 cycles, the cathode delivered capacities of 118 and 73 mAh g −1 at the high current densities of 5 C and 20 C, respectively, displaying superior rate performances. The TH-COF/rGO electrode exhibited high capacity and stability, making it a promising cathode material for the next generation LIBs.
研究领域:
材料科学
·
能量存储
·
电化学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Yusheng Gao,Aiqun Kong,Mao Peng,Ye Lv,Menghui Liu,Wei Li,Jinli Zhang,Yan Fu
It is particularly challengeable to achieve C=O selectivity for Pd catalysts in thermal catalytic hydrogenation of cinnamaldehyde (CAL). This work offers a new electrochemical strategy that enables an unexpected switch toward C=O bond for CAL hydrogenation, based on the specific interaction between CAL and electrolyte-modulated Pd surface. Under galvanostatic electrolysis, guanosine 5′-monophosphate-modulated Pd electrode affords a record cinnamyl alcohol (COL) selectivity of 90.3% in neutral catholyte with no sacrifice of CAL conversion, showing the faradaic efficiency of 68.2%. It is of great interest to find that the aromatic moiety of CAL determines the preferential activation toward C=O bond over Pd surface under electric field. It is reported for the first time that selective hydrogenation of α, β-unsaturated aldehydes can be altered by electrochemical environment located between Pd electrode and surrounding electrolyte involving alkali cation along with organic solvent.
研究领域:
电化学
·
催化
·
有机化学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Zhen Pu,Jianwei Qin,Xiaoguo Fu,Ruizhi Qiu,Bin Su,Maobing Shuai,Fang Li
Fundamental investigation of metal–CO interactions is of great importance for the development of high-performance catalysts to CO activation. Herein, a series of side-on bonded mononuclear lanthanide (Ln) oxocarbonyl complexes OLn(η2-CO) (Ln = La, Ce, Pr, and Nd) have been prepared and identified in solid argon matrices. The complexes exhibit uncommonly low C–O stretching bands near 1630 cm–1, indicating remarkable C–O bond activation in these Ln analogues. The η2-CO ligand in OLn(η2-CO) can be claimed as an anion on the basis of the experimental observations and quantum chemistry investigations, although the CO anion is commonly considered to be unstable with electron auto-detachment. The CO activation in OLn(η2-CO) is attributed to the photoinduced intramolecular charge transfer from LnO to CO rather than the generally accepted metal → CO π back-donation, which conforms to the traditional Dewar–Chatt–Duncanson motif. Energy decomposition analysis combined with natural orbitals for chemical valence calculations demonstrates that the bonding between LnO and η2-CO arises from the combination of dominant ionic forces (>76%) and normal Lewis “acid–base” interactions. The fundamental findings provide guidelines for the catalyst design of CO activation.
研究领域:
无机化学
·
物理化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Xiaofei Liu,Daiyu Song,Yunyun Liu,Zhao Huang,Xinyao Wang,Kezhi Wang,Yuxin Yang,Yihang Guo
The cleavage of C–O bonds in biomass-derived carbohydrates is of great significance for the conversion of biomass to chemicals and fuels. We demonstrated that various F127-directed covalent triazine frameworks functionalized by sulfonic acid-based ionic liquids ([C 3 N][OTf]-FCTF) were synthesized by a two-step synthesis process. The interesting morphology of spherical nanofiber of the [C 3 N][OTf]-FCTF(0.25)-10 catalyst was obtained by carefully adjusting the usage of both F127 and ethanol in the synthetic system. The 5-hydroxymethylfurfural synthesis reaction parameters of were first optimized using the [C 3 N][OTf]-FCTF(0.25)-10 via response surface methodology. The [C 3 N][OTf]-FCTF(0.25)-10 exhibited high catalytic activity, and outperformed other CTF-based catalysts with different morphologies and commercial solid acids in the conversion of carbohydrates (e.g., fructose, inulin, sucrose and honey). This is due to the advantages of the loose spherical nanofiber, the rich N-containing units, the suitable Brønsted acid nature and the adjacent acid-base pairs on the surface of the catalyst. The high Brønsted acidity of [C 3 N][OTf]-FCTF(0.25)-10 played a positive role in the selective synthesis of levulinic acid from carbohydrates. The theoretical calculations demonstrated that discrepancies in electron cloud distribution between constructed acid-base pairs and N-rich groups in the catalyst could facilitate the cleavage of C–O bonds in fructose molecules. The Fukui function combined with experimental results elucidated the reaction pathways. The robust interaction between –[C 3 N][OTf] groups and frameworks ensured the excellent reusability of [C 3 N][OTf]-FCTF catalysts. This study will provide a novel approach for synthesizing CTF-based solid acids with controllable morphology, enabling the high-value utilization of carbohydrates.
研究领域:
催化化学
·
材料科学
·
绿色化学
·
生物质转化
·
有机合成
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
Chem Catalysis
·
2023
·
IF 9.4
Rong Wang,Yue Peng,Jane Chung,Zhen Chen,Xiyang Wang,Haibo Yin,Yimin A. Wu,Jingshan Luo,Junhua Li
Summary The electrocatalytic reduction of CO 2 is an attractive method for reducing greenhouse gases and producing chemical feedstocks. However, the activation of C=O bonds limits the reaction kinetics; therefore, understanding the mechanism of C=O bond activation can guide the design of high-performance catalysts. Here, we investigate the C=O bond activation mechanism during the electroreduction of CO 2 to CO on ZnO. Using in situ experimental techniques and quantum chemical calculations , we find that defects in ZnO promote the formation of Zn–ZnO x interfaces during CO 2 reduction, which mediates an intimate-junction exciton state by the metal semiconductor heterophase. This promotes the formation of CO 2 radicals, exposing electron donation centers for CO 2 adsorption and redox centers for cleaving stable C=O bonds. The internal electric field generated by the heterojunction enhances the initial C=O activation by facilitating the interaction between the metalized Zn d-orbital and the O π -orbital in CO 2 .
研究领域:
电化学
·
材料科学
·
催化
·
表面科学
✓ 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）