LANGMUIR
·
2021
·
IF 3.882
Chaoyue Xiong,Guodong Xue,Lijun Mao,Lianghong Gu,Chao He,Yonghao Zheng,Dongsheng Wang
Understanding the relationship between chemical structure and photoswitching property of donor–acceptor Stenhouse adducts (DASAs) is necessary for developments and applications of the novel photoresponsive molecule. In the current work, we demonstrated a close relationship between the length of carbon spacer and photoswitching property of DASAs. A series of DASAs with barbituric acid substituted electron-withdrawing part and N-methylaniline substituted electron-donating part were synthesized. With shortening the carbon spacer between the phenyl and amine groups in the electron-donating part, the efficiency and rate of the light-induced linear-to-cyclic isomerization are improved in all the test solvents. The molecular energy variation during the isomerization process was investigated by density functional theory calculation to further understand the mechanism. This work provides a reliable carbon spacer strategy to control the photoswitching behavior of DASAs using chemical methods.
研究领域:
有机化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Chengyu Zhang,Zhisheng Yu,Xiangyang Wang,Bobo Wang
In this study, a novel γ-Fe 2 O 3 /biochar (BF γ ) composite by a plant in-situ enrichment and one-step pyrolysis strategy was prepared, which was applied as a photocatalyst to activate peroxymonosulfate (PMS) for the degradation of p-chlorophenol (4-CP) under visible light irradiation (BF γ /PMS/Vis) system. The characterization results exhibited that γ-Fe 2 O 3 with localized carbon doping was evenly embedded in biochar during the pyrolysis. BF γ exhibited better photoresponse properties than biochar (BC) and γ-Fe 2 O 3 . The removal efficiency of this system for 4-CP reached 96.41% under optimal conditions. This system showed high removal efficiency with a wide pH range (3.0–13.0) and under conditions of different organic pollutants . It also showed strong resistance to interference with co-existing inorganic ions and humic acid (HA). Electron paramagnetic resonance (EPR) and radical scavenging experiments revealed that the reactive oxygen species (ROS) in this system included SO 4 - ·, ·OH, ·O 2 - and 1 O 2 . The density functional theoretical (DFT) calculations further revealed the promotion of localized carbon doping in γ-Fe 2 O 3 on electron transfer and photoresponse, including C-O bond (d=1.29 Å), C-Fe bond (d=1.80 Å) and band gap value (E gap < 0.72 eV). This study provides new insights into constructing environmentally-friendly catalysts and the possibility of the solid waste recycling for other wetland plants.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2021
·
IF 3.882
Aling Chen,Qingfeng Yi,Kuang Sheng,Yuebing Wang,Jiangchuan Chen,Qiaoli Zhang,Kaiwen Xiang,Guanghua Tan
Development of high-efficiency oxygen reduction reaction (ORR) catalysts under neutral conditions has made little research progress. In this work, we synthesized a three-dimensional porous N/P codoped carbon nanosheet composites (CNP@PNS) by high-temperature thermal treatment of dicyandiamide, starch, and triphenylphosphine and subsequent porous structure-making treatment using the NaCl molten salt template. In the neutral solution, the electrocatalytic performance of the CNP@PNS-4 catalyst exhibits an onset potential of 0.98 V (vs reversible hydrogen electrode) and a half-wave potential of 0.91 V for ORR, which greatly surpasses commercial Pt/C (40%). Three kinds of neutral metal–air batteries (Zn–air, Al–air, and Fe–air) using the prepared samples as cathodic catalysts were constructed, corresponding to the maximum power density of 120.2, 78.3, and 18.9 mW·cm–2, respectively. Also, they reveal outstanding discharge stability under different current densities. The density functional theory calculation depicts the reduction of the free energy of the determining step and subsequent decline of the overpotential for ORR.
研究领域:
材料科学
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电化学
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能源科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xiaolei Shi,Weibin Ma,Wei Chen,Xuan Tao,Chunxiao Gong,Shuai Gao,Lujiang Xu,Zhen Fang
Phenol is a typical toxic and persistent pollutant in wastewater, requiring efficient and recyclable adsorbents for its removal. In this study, Fe–N co-doped biochar was synthesized through four preparation routes combining KOH activation and FeCl 3 -NH 3 modification, and its phenol adsorption behavior and formation mechanism were systematically investigated. The biochar exhibited specific surface areas of 400–900 m 2 /g and N contents of 1.85–3.92 at.%, enabling the formation of Fe 2 O 3 , Fe 3 O 4 , and Fe-N x species. Among the samples, the biochar prepared at 800 °C via activation and soaking–drying achieved the highest phenol adsorption capacity (263.09 mg/g). Adsorption followed the Freundlich isotherm and pseudo-second-order kinetic model, indicating multilayer chemical adsorption. Cycling experiments revealed that Fe 2 O 3 and Fe 3 O 4 were easily detached, whereas Fe-N x remained stable, maintaining 76 % adsorption capacity after five cycles. DFT calculations further confirmed the strong anchoring of Fe ions by N-doped micropores and the thermodynamic stability of Fe-N x structures. This work demonstrates a simple and effective approach for preparing stable Fe-N biochar and provides mechanistic insight into its enhanced phenol adsorption.
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产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Xue Qi,Hongmin Gao,Lei Wu,Yang Zhou,Hehua Zhang,Dong Chang,Hongzhi Pan
Accurate and sensitive detection of the neurotransmitter dopamine (DA) plays a significant role in medical diagnosis and human health assessment. Herein, an electrochemical sensing platform for ultrasensitive determination of DA was constructed based on porous Co 3 O 4 nanocubes anchored to three-dimensional Ti 3 C 2 MXene-reduced graphene oxide aerogel (Co 3 O 4 /3D MX-rGO). The 3D MX-rGO aerogel with a high specific surface prevents aggregation of Co 3 O 4 nanocubes and exposes more active sites, resulting in excellent electrocatalytic activity and outstanding sensing properties. The electrochemical reaction kinetic was investigated in detail, a possible sensing mechanism was proposed, and the interaction mechanism between the composites and DA was revealed combined with density functional theory (DFT) calculations. Under optimized experimental conditions, the sensor developed using Co 3 O 4 /3D MX-rGO modified glassy carbon electrodes (GCE) exhibited low detection limits (40 nM) in the range of 0.1–300 μM for DA with good selectivity, reproducibility, and stability. The sensor has been successfully use to detect DA in human serum and urine samples with recoveries of 95.3 %-103.7 %, which has great potential for practical applications.
研究领域:
生物医学工程
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材料科学
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分析化学
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产品关联
DOI
高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 12
·6897-6908
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IF 4.21
Guo Weihao,Zuo Minghui,Zhao Jian,Li Chao,Xu Qiaoliang,Xu Chunzhao,Wu Hongfeng,Sun Zhizhong,Chu Wenyi
A series of Brønsted–Lewis acidic di-cationic ionic liquids ( BLAILs ) were synthesized and the catalytic properties of glucose conversion to 5-hydroxymethylfurfural (5-HMF) were investigated. The experimental results showed that the ionic liquid with aluminum trichloride as Lewis acid anion ( BLAIL - 5 ) exhibited good catalytic performance. Under the best reaction conditions, the yield of the glucose conversion into 5-HMF and 5-EMF were 71% and 66%, respectively. In addition, the yield of cellulose to 5-HMF is 41%. The optimized catalytic system could be reused for 5 times without significant catalytic performance loss. In addition, the mechanism of BLAIL - 5 promoting glucose conversion to 5-HMF was studied by density functional theory calculation (DFT).
研究领域:
化学工程
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催化化学
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生物质转化
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Jingwei Wang,Yaoyong Dong,Xuejun Zheng,Bei long,Hui Ling,Long Xie,Zhenhua Xiang,Wenyuan He
This report reveals that the hydrogen evolution activity of VS 2 can be effectively strengthened by inducing the surface charge redistribution of VS 2 via P non-metal doping. The XRD, TEM, GPA, EDS and XPS characterizations confirm that the P atoms are successfully doped into the VS 2 /CC matrix by substituting S atoms, resulting in lattice tensile strain and charge redistribution. The optimal P-doped VS 2 on carbon cloth (P-VS 2 /CC) exhibits a low overpotential of 274 mV at − 50 mA cm −2 and a small Tafel slope of 65.4 mV dec -1 , much lower than those of VS 2 /CC counterpart (622 mV and 120.1 mV dec −1 , respectively). Moreover, the P-VS 2 /CC delivers a long-term stability for 55 h without decay at 10 mA cm −2 , outperforming the VS 2 /CC. Density functional theory calculations suggest that P doping can induce the charge transfer from S and V to nearby P atoms, resulting in the decrease of hydrogen adsorption free energy at the S and V sites and the increase of total density of states at the Fermi level, thus far super hydrogen evolution activity. This work provides a hopeful new route for strengthening the HER activity of VS 2 , and offers a new perspective for developing advanced transition-metal chalcogenides electrocatalysts.
研究领域:
材料科学
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电化学
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纳米催化
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能源材料
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计算材料学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Tingting Tang,Yutao Cao,Min Li,Shuo Cui,Ying Wu,Zhize Yu,Wei Cui,Hong Zhao
The rational construction of highly efficient electrocatalysts toward the hydrogen evolution reaction (HER) in alkaline electrolytes is critical for renewable energy technologies, but still challenging in seawater electrolysis at ampere-level current density. Herein, we design a nanoarray composite catalyst Ni 2 P@W-MoO 2 through one-step hydrothermal and post-phosphidation, which shows excellent catalytic activity for hydrogen evolution in all alkaline, simulated seawater and seawater electrolytes at ampere-level current density, with low overpotentials of 328, 352 and 364 mV, respectively. Furthermore, an overall urea-assisted water splitting electrolyzer obtained by using Ni 2 P@W-MoO 2 as the bifunctional catalyst can deliver a current density of 10 mA cm −2 at a cell voltage of 1.36 V and operate stably for 100 h. In situ ATR-FTIR monitors the dynamic adsorption behavior of the important intermediate *OH on the surface of electrocatalysts. A series of density functional theory calculations further uncover the incorporation of W ameliorates the microenvironment of the MoO 2 and decreases the H 2 O/*OH adsorption/dissociation energy barriers, simultaneously optimizing the H* Gibbes free energy on the Ni 2 P, which achieves superior electrochemical water splitting performance. This work breaks through the proton-deficient dilemma of the alkaline HER at ampere-level current density and provides new insights into the design of cost-efficiency and environmentally friendly transition metal-based catalysts.
研究领域:
电化学
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材料科学
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能源化学
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纳米催化
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可持续能源技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Quanxing Zhang,Caoying Kang,Zhaozhe Li,Kerui Hua,Dongpei Zhang,Wei Yu,Xin Jin,Chaohe Yang
Glutaric acid, a C 5 dicarboxylic acid, servers as an essential monomer in nylon industry. Currently, it is primarily obtained as a byproduct of adipic acid production. Green synthesis of glutaric acid from bio-resources remains a grand challenge. Here, we present a two-step synthesis of glutaric acid from furfural via cyclopentanone as the key intermediate. In the first step, a series of Ni modified CuO x catalysts derived from HKUST-1 (Cu) displays a record conversion rate (20.8 h −1 at 140 ℃) in converting furfural to cyclopentanone, with 99.8 % conversion of furfural and 87.4 % selectivity to cyclopentanone. The d-d orbital coupling between Ni and Cu through the oxygen bridge bond leads to an upshifted d band center of Cu sites, inducing the σ-bonding between the e g orbital of the electron-deficient Cu 2+ and C=O bond of furfural. In the second step, the C=O bond of cyclopentanone can be activated effectively over electron-rich Cu 2+ sites of HKUST-1 (Cu). The oxidation of cyclopentanone to glutaric acid was achieved on heterogeneous catalyst for the first time, with 40 % and 17.6 % yield of glutaric and succinic acids, respectively. The reaction mechanism has also been proposed. DFT calculation has revealed that 1,1,2-trihydroxy-cyclopentane is an important intermediate product, with proton removal to form C-O· radical as the rate-determining step. This work provides insights into the synthesis of bio-glutaric acid through a chemocatalytic route.
研究领域:
催化
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绿色化学
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有机合成
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2025
·
IF 6.3
Juncheng Jiang,Hang Yao,Jialei Huang,Zhiquan Chen,Lei Ni,Yong Pan
Background: Nitro-m-xylene (NMX) is a critical raw material and intermediate widely used in the synthesis of fine chemical products and energetic materials. A clear understanding of the thermal hazards and safety performance of NMX is especially critical for practical applications in chemical processes. Methods: Calorimetric experiments combined with theoretical chemical calculations were applied to investigate the thermal decomposition and kinetic behavior of NMX. Significant findings: The average apparent activation energies for the decomposition of NMX, the nitration products of m-xylene, calculated using the DAEM, Starink and Friedman methods were 141.1 kJ/mol, 141.4 kJ/mol and 144.9 kJ/mol, respectively. The most probable decomposition mechanism functions were determined by the master plots method at conversions of 0.05–0.50 and 0.50–0.95 for modes A4 and F2, separately. Furthermore, calculations of thermal safety and thermodynamic parameters revealed the excellent thermal stability of the nitration products, which require an external heat source to trigger decomposition. The C-NO 2 bond was identified as a possible initial decomposition site for 4-NMX by theoretical bond order and dual descriptor analysis. The possible decomposition pathways for 4-NMX were deduced by density functional theory, and alkyl compounds were the main gaseous products, followed by small molecules containing O and N.
研究领域:
化学安全
·
热分析
·
计算化学
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反应动力学
·
能量材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Qi Xue,Xin-Yu Bai,Yue Zhao,Ya-Nan Li,Tian-Jiao Wang,Hui-Ying Sun,Fu-Min Li,Pei Chen,Pujun Jin,Shi-Bin Yin,Yu Chen
Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen (H 2 ) production from acidic water electrolysis. Herein we report the one-pot precise synthesis of ultrafine Au core-PtAu alloy shell nanowires (Au@Pt x Au UFNWs). Among them, Au@Pt 0.077 Au UFNWs exhibit the best performance for formic acid oxidation reaction (FAOR) and hydrogen evolution reaction (HER), which only require applied potentials of 0.29 V and −22.6 mV to achieve a current density of 10 mA cm −2 , respectively. The corresponding formic acid electrolyzer realizes the electrochemical H 2 production at a voltage of only 0.51 V with 10 mA cm −2 current density. Density functional theory (DFT) calculations reveal that the Au-riched PtAu alloy structure can facilitates the direct oxidation pathway of FAOR and consequently elevates the FAOR activity of Au@Pt 0.077 Au UFNWs. This work provides meaningful insights into the electrochemical H 2 production from both the construction of advanced bifunctional electrocatalysts and the replacement of OER.
研究领域:
材料科学
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电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2020
·
IF 4.049
Xiaowei Sun,Wenhua Ji,Shenghuai Hou,Xiao Wang
Trifluoromethyl covalent organic framework (CF 3 -COF) is facilely synthesized at room temperature using for solid-phase microextraction (SPME). The CF 3 -COF coating displays an improved extraction performance for per- and polyfluorinated alkyl substances (PFASs) comparing to amorphous polymer coating, non-contained fluorine covalent organic framework coating and commercially available SPME coating. The fluorine affinity of trifluoromethyl in CF 3 -COF for PFASs is demonstrated using the density functional theory calculation. Following the microextraction with CF 3 -COF-coated fiber, the targeted PFASs are eluted with 1 mL acetonitrile and quantified by ultrahigh performance liquid chromatography tandem mass spectrometry. The low limits of detection are 0.1–0.7 pg g −1 for milk and 0.2–0.8 pg g −1 for milk powder, suggesting the outstanding sensitivity. The precision for the method ranges between 2.9 and 9.9%. The fiber-to-fiber repeatability is in the range of 4.2–9.5%. Under the optimum conditions, the relative recoveries are 91.0–110% with RSDs ≤ 10% for milk and 89.8–111% with RSDs ≤ 10% for milk powder.
研究领域:
分析化学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）