ACS Catalysis
·
2025
·
IF 13.1
Tao Wang,Qiao Yu,Zhilin Chen,Chao Xiao,Shuming Peng
The active phase for methane combustion is still in debate. Low-temperature CO-FTIR spectroscopy was used to probe the working surface state on a series of Pd/Al2O3 (PdAl) and Pd/silicalite-1 (PdSil) catalysts with different starting states: oxidized, reduced (R), reoxidized (Ro). The surface of prereduced PdAl (Pd0) is transformed to an oxidized state (PdOx) with a CO stretching vibration (νCO) at ∼2157 cm–1 when it is aged in the methane oxidation mixture. The aging-induced transformation from Pd0 to PdOx occurred at 250 °C or above. Although PdSil has multiple kinds of PdOx entities, prereduced PdSil also transformed into PdOx. For PdAl(4)-R-A250, XRD patterns suggest weak bulk oxidation of Pd0 at 250 °C, XPS spectra indicate 28% of surface Pd0 atoms are oxidized, but CO-FTIR spectra confirm all the “top surface” Pd0 atoms are oxidized. It demonstrates the advantage of CO-FTIR spectroscopy in probing the top surface state. Finally, a direct correlation between operando FTIR spectroscopy and low-temperature CO-FTIR spectroscopy was established. Operando FTIR spectra over PdSil during methane oxidation at 250 °C gives two bands at 2124 cm–1 (CO–Pd+) and 2161 cm–1 (CO–Pd2+). After cooling in nitrogen, CO-FTIR spectra give two similar bands at 2134 cm–1 and 2157 cm–1. The “working surface state” can be preserved in CO-FTIR. For PdAl(4), operando FTIR spectra at 250 and 300 °C give no bands of adsorbed CO. Adding CO into the methane oxidation mixture resulted in a single CO–Pd2+ band at 2163 cm–1, which is in accord with their CO-FTIR spectra. For operando FTIR spectroscopy, the observation of the bands of adsorbed CO depends on the accumulation of the CO intermediates, but their accumulation is limited to reaction temperatures below 300 °C and to PdSil (not PdAl). These limitations make low-temperature CO-FTIR spectroscopy more general and sensitive.
研究领域:
催化化学
·
材料科学
·
环境化学
·
光谱学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Fengdong Qu,Wenan Shang,Dongting Wang,Shiyu Du,Tiju Thomas,Shengping Ruan,Minghui Yang
Multishell, stable, porous metal-oxide microspheres (Ni–Co oxides, Co3O4 and NiO) have been synthesized through the amorphous coordination polymer-based self-templated method. Both oxides of Ni and Co show poor selectivity to xylene, but the composite phase has substantial selectivity (e.g., Sxylene/Sethanol = 2.69) and remarkable sensitivity (11.5–5 ppm xylene at 255 °C). The short response and recovery times (6 and 9 s), excellent humidity-resistance performance (with coefficient of variation = 11.4%), good cyclability, and long-term stability (sensitivity attenuation of ∼9.5% after 30 days and stable sensitivity thereafter) all show that this composite is a competitive solution to the problem of xylene sensing. The sensing performances are evidently due to the high specific surface area and the nano-heterostructure in the composite phase.
研究领域:
材料科学
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化学传感器
·
纳米技术
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yan Chen,Yufan Liu,Huizhen Jin,Xinyue Wang,Guowen Wang,Hongchao Ma,Vadivel Subramaniam,Krishnamoorthy Ramachandran,Xinghui Liu
Antibiotic drugs are biotoxic and difficult to degrade, causing irreversible effects on aquatic environment and human health. The photoelectrocatalytic (PEC) process is regarded as a promising strategy for simultaneously addressing environmental pollution and the energy crisis. Herein, a plum tree-type composite semiconductor photoanode MnOx@Co/NC-x with core-shell heterostructures was constructed to evaluate the PEC activity for sulfamethoxazole (SMX). The synergistic effects of Co nanoparticles, a high content of graphitic N, an open framework, and interfacial structures played a decisive role in improving the PEC activity of the MnOx@Co/NC-x system. The engineered micro-nano structure significantly improved the specific surface area and conductivity of electrode materials, and promoted the diffusion of electrolyte. Among them, MnOx@Co/NC-500 photoanode exhibited the best performance (reached 98.92% in 50 min), cyclic stability and repeatability. The results showed that it was feasible to construct a high-performance heterostructural interface for pollutant treatment based on micro-nano structure regulation and valence band matching.
研究领域:
环境催化
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材料化学
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环境污染治理
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纳米材料
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电化学
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光化学
·
药物降解
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 17
·9435-9444
·
IF 14.511
Qingshan Zhao,Wanxin Ni,Xiaojie Tan,Fengliang Cao,Tengfei Liu,Hao Huang,Zhinian Cheng,Yiwen Li,Shuwei He,Hui Ning,Mingbo Wu
Selective hydrogenation of nitroarenes to corresponding anilines is one of the most important processes in the chemical industry, which still suffers from lack of efficient catalysts with both high activity and selectivity. Herein, a reinforced single-atom Co catalyst (Co–N–CNS–Th) was rationally fabricated through a novel “Trojan horse” strategy for boosting selective hydrogenation of nitroarenes. The cobalt salt precursor is confined in a mixed molten salt (KCl + CaCl2) via recrystallization and gradually released when reaching the melting point, which can efficiently achieve atomic Co–N4 moieties accommodated in micropore defect-rich carbon nanosheets. The prepared Co–N–CNS–Th catalyst showed superior hydrogenation activity and selectivity (yield of >99%; overall TOF of 169.8 h−1) towards a series of functionalized nitroarenes under mild reaction conditions, as well as remarkable stability and reusability, standing out among the reported cobalt-based catalysts. The experimental results and DFT calculations reveal that the robust atomically dispersed Co–N4 active sites located near the edge of micropore defects can significantly accelerate the adsorption and activation of hydrogen and nitro groups, accounting for the prominent catalytic performance. This work opens a feasible avenue for the development of advanced single-atom catalysts towards selective hydrogenation of nitroarenes and beyond.
研究领域:
催化化学
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材料科学
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理论计算化学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Xiaowen Su,Shan Wu,Xiaoxing Long,Yan Shi,Qi Pan,Jixin Su
Preventing climate change and achieving carbon neutralization depend on strengthening the carbon cycle in industry and limiting carbon emissions to ambient air. Our aim is to reduce CO 2 to valuable CO by gas-solid photo-catalytic reduction under sunlight. We prepared catalysts by one-step synthesis with graphene oxide (GO) and ZnO, surface modified with a monolayer of sulfonated cobalt phthalocyanine (CoPcS), which were calcined to obtain photocatalyst samples containing Co(II), ZnO and reduced graphene oxide (rGO). Results of TEM, SEM-EDS, XRD, XPS, PL and ESR revealed that the photocatalyst samples possessed a hybrid layer microstructure, heterojunction, and excellent electron-hole pair separation. Evaluation of the photocatalytic reduction reactivity showed that CO selectivity reached 96.2–99.0% and top CO yield was 26.15 µmol.g −1 .h −1 .
研究领域:
环境科学
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材料科学
·
化学工程
·
光化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2020
·
IF 2.304
Muhammad Usman,Haojie Yu,Li Wang,Jianguo Qian,Xuefeng Li,Amin Khan,Kaleem-ur-Rehman Naveed,Ahsan Nazir,Tarig Elshaarani,Shah Fahad
A series of copolymers of poly(2-(methacryloyloxy) ethyl ferrocene carboxylate- co -methacrylic acid)s (P(FHEMA- co -MAA)s) were synthesized as burning rate catalysts (BRCs). Their structures were verified using proton nuclear magnetic resonance ( 1 H NMR) and Fourier transforms infrared (FT-IR) spectroscopy. The electrochemical behavior of P(FHEMA- co -MAA)s was investigated by cyclic voltammetry (CV). The CV results indicated that P(FHEMA- co -MAA)s showed redox behavior. Anti-migration test proved that P(FHEMA -co- MAA)s possesses better anti-migration properties than ferrocene (Fc) and 2, 2-bis (ethylferrocenyl) propane (Catocene). The burning rate (BR) catalytic effect of P(FHEMA -co- MAA)s on thermal decomposition of AP was examined through thermogravimetry (TG) and differential thermogravimetry (DTG). P(FHEMA -co- MAA)s were found to have high catalytic effects in accelerating thermal decomposition of ammonium perchlorate (AP).
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2024
·Vol. 137
·期 3
·1535-1552
·
IF 1.7
Feng Shangzhen,Zhou Hantao,Jiang Huanjin,Yang Jie,Chen Jixiang
Herein, the Ni–Co alloy supported on TiO 2 catalysts were prepared by sol–gel method assisted with Polymethyl Methacrylate (PMMA) template, and they were tested for in situ aqueous phase hydrodeoxygenation (HDO) of methyl palmitate to hydrocarbons using methanol as hydrogen donor. It has been found that the introduction of PMMA decreases the Ni–Co alloy particles size, reduces the metal-support interactions (SMSI), constructs the mesopores and enlarges the mesopore size. Also, the Ni–Co alloy particles can be partially embedded in TiO 2 , beneficial to the catalyst stability since the sintering and leaching of the Ni–Co alloy particles can be suppressed under hydrothermal condition. In the in situ HDO of methyl palmitate, the main deoxygenation pathway is decarboxylation/decarbonylation on the Ni–Co alloy catalysts. The catalysts prepared with PMMA exhibits higher activity than that without PMMA, giving the pentadecane yield of 86.2% at 310 °C. This is ascribed to their more exposed active sites and wider mesopores. Moreover, the catalyst is not obviously deactivated during five reactions.
研究领域:
催化
·
化学工程
·
材料科学
·
环境科学
·
有机化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Ming Yin,Li Zhang,Xiuxia Wei,Yiwei Sun,Shuyan Qi,Yan Chen,Xinxin Tian,Jingxuan Qiu,Dongpo Xu
This work is carried out by the synergy of Co/Ni-Bio-MOF and noble metal Au-doped coral-like ZrO 2 . A novel electrochemical aptamer sensor (aptasensor) for measuring kanamycin (Kan) was developed by using ZrO 2 @Au as an amplification platform for electrochemical aptasensors. ZrO 2 @Au was strategically used to significantly reduce the Differential Pulse Voltammetry (DPV) response by hindering electron transfer at the working electrode surface. When Kan is recognized by the ZrO 2 @Au-linked aptamer, it is disconnected from the complementary sequence attached to the Co/Ni-Bio-MOF due to the applied force, thereby disengaging from the electrode. This results in the removal of obstacles to electron transfer, enabling signal amplification. This electrochemical sensor exhibits good linearity from 10 μM to 1000 μM. It has a detection limit of 0.037 μM and has excellent stability (RSD = 0.14–0.21%), reproducibility (RSD = 0.079–0.63%) and selectivity.
研究领域:
分析化学
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电化学
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生物传感器
·
环境监测
✓ 已验证
DOI
高影响因子
Materials
·
2024
·Vol. 17
·期 5
·1200
·
IF 3.1
Wei Tong,Weiqiang Wang,Xiayu Leng,Jianli Song
To enhance the comprehensive performance of solid oxide fuel cells (SOFCs) ferritic stainless steel (FSS) interconnectors, a novel approach involving composite electrodeposition and thermal conversion is proposed to prepare Ni-doped Co-Mn composite spinel protective coatings on FSS surfaces. The process involves the composite electrodeposition of a Ni-doped Co-Mn precursor coating, followed by thermal conversion to obtain the Co-Mn-Ni composite spinel coating. Crofer 22H was used as the substrate and orthogonal experiments were designed to investigate the influences of deposition solution pH, stirring rate, cathode current density, and the element content of Mn and Ni on the surface morphology and properties of the composite coatings, respectively. The characterization of the prepared coatings was conducted through macroscopic and microscopic morphology observations of the component surface, energy dispersive spectroscopy (EDS) analysis, and area specific resistance (ASR) testing, etc. Finally, the optimized composite electrodeposition parameters and the Mn-Ni content ratio in the solution were obtained. Experimental results indicated that the composite spinel coating prepared with the optimized process parameters exhibited excellent adhesion to the substrate, and the diffusion and migration of Cr element has been effectively inhibited. Compared with the substrate, the ASR of the coated components has also been decreased simultaneously, which provided an effective method for the surface modification of SOFC FSS interconnectors.
研究领域:
材料科学
·
电化学
·
能源材料
·
表面工程
✓ 已验证
DOI
PubMed
高影响因子
Biomaterials Advances
·
2025
·
IF 6
Chen Wang,Yin Li,Xiaoxue Shen,Shiwei Xiao,Huiying Du,Qianye Zhao,Ying Wang,Qiangtao Zhang,Shuxin Wen
Background Patients with locally advanced head and neck squamous cell carcinoma (HNSCC) exhibit poor survival due to tumor microenvironment (TME) barriers and systemic toxicity of chemo-immunotherapy associated with chemo-immunotherapy. Methods An injectable thermoresponsive hydrogel was engineered by crosslinking D-α-tocopheryl polyethylene glycol succinate (TPGS) with Na₂CO₃ (15 % w/v TPGS: 9 % w/v Na₂CO₃). This platform co-encapsulated doxorubicin-loaded nanoparticles (DOX NP) synthesized via PEI-cis-aconitic acid conjugation and CpG-loaded adjuvant nanoparticles (CpG NP) prepared through genipin-mediated PEI crosslinking. The hydrogel exhibited rapid temperature-triggered gelation, shear-thinning injectability, and a macroporous architecture that enabled dual drug retention and immune cell infiltration. Results In vitro , the hydrogel provided the sustained release of DOX NP with pH-responsive acceleration in acidic TME. In vivo , localized delivery of Gel-DOX NP-CpG NP significantly suppressed tumor growth ( p < 0.05) and enhanced cytotoxic CD8 + T-cell infiltration in TME (3.1-fold) and spleens (2.4-fold). RNA sequencing revealed 88 immune-related differentially expressed genes, including downregulated immunosuppressors and enriched cytokine pathways. Conclusion This TPGS/Na₂CO₃ hydrogel platform coordinates chemotherapy-induced immunogenic cell death (DOX NP) with CpG-driven innate immunity, overcoming TME barriers to enhance localized and systemic anti-tumor responses in HNSCC.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Ming-feng Sun,Ting Wang,Li-guang Wu,Yu-xing Wang
This study attempted to enhance the permeation and antifouling performance of polyvinylidene fluoride (PVDF) ultrafiltration membranes. Reverse microemulsion containing cobalt and iron (Co–Fe) bimetallic hydroxide nanoparticles was blended with the PVDF membranes to construct a novel PVDF hybrid membrane. The permeation performance, antifouling property, and long-term operational stability of the hybrid membranes were evaluated via ultrafiltration process of water flux and bovine serum albumin (BSA) rejection. Structural characterization showed that the protection endowed by reverse microemulsion made the hydroxide nanoparticles to distribute uniformly in the PVDF polymeric matrix. The introduction of well-distributed bimetallic hydroxide nanoparticles substantially improved the pore structures and hydrophilicity of the PVDF hybrid membranes, thereby enhancing their permeation performance and antifouling property. The optimal water flux of the PVDF hybrid membranes (MD-10) reached 328 L·m −2 ·h −1 and was 5.4-fold higher than that of neat PVDF. Moreover, the MD-10 membrane had a high a high BSA rejection rate (91.04%). After four cycles of successive fouling-cleaning processes, the water flux of the MD-10 membrane still exceeded 160 L·m −2 ·h −1 and was fourfold higher than that of neat PVDF. However, excessive amounts of the microemulsion could not be uniformly mixed with the PVDF membranes, thereby decreasing the permeation and antifouling performance of the PVDF hybrid membranes.
研究领域:
膜科学
·
纳米技术
·
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Zihao Dong,Yajuan Qu,Yuyang Jiao,Ke Xue,Wenguang Zhu,Hai Liu,Jianguang Qi,Yinglong Wang
A series of poly(1-vinyl-3-methylimidazole dimethyl phosphate- co -N-isopropylacrylamide) oligomers was synthesized by reversible addition-fragmentation chain transfer polymerization. The co-oligomers exhibited a pH-tunable lower critical solution temperature (LCST) phase transition in aqueous solutions. By changing the pH of the aqueous solution (HCI), the hydrogen bonding between the internal molecules of the co-oligomers and water molecules was weakened, which effectively reduced the cloud-point temperature. Poly(1-vinyl-3-methylimidazole dimethyl phosphate- co - N -isopropylacrylamide) oligomers exhibit an upper critical solution temperature (UCST) type of phase transition in an ester solution, which is associated with the formation and breaking of hydrogen bonds within the co-oligomers molecules. FT-IR analysis revealed the effect of temperature on hydrogen bonding between the functional groups. Energy decomposition, Electrostatic Potential (ESP), Atoms-in-Molecules (AIM), and Interaction region indicator (IRI) analyses demonstrated the presence of hydrogen bond donors N–H and imidazole ring C–H, and hydrogen bond acceptors C = O and P = O in the co-oligomers. The sites of hydrogen bonding between the co-oligomers and the solvent molecules as well as intermolecular forces were found to be the main factors contributing to the LCST/UCST-type phase transition.
研究领域:
高分子化学
·
物理化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）