FUEL
·
2025
·
IF 7.5
Xiaohui Wang,Zhilong Cheng,Bingrong Liu,Huiyi Liu,Xin Fang,Ruiqi Chai,Lishuang Ma,Yuchao Lyu,Jianye Fu,Xinmei Liu
Methane dehydroaromatization (MDA) was a promising technology for the synthesis of high value-added aromatics through natural gas. Fe/ZSM-5 catalysts were widely used in MDA reaction. However, its catalytic mechanism remained ambiguous. In this work, a novel one-pot strategy was developed for the preparation of Fe/ZSM-5 catalysts, which can delicately control the iron species and acidic property of Fe/ZSM-5 catalysts. In-situ DRIFTS and DFT calculation demonstrated that MDA followed a bifunctional mechanism and the second C–H bond breaking process of CH 4 was the rate-determining step, where methane underwent coupling and dehydrogenation at the iron active sites to generate intermediate species (ethylene), and Brønsted acid sites played a key role in determining the selectivity of aromatics. Moreover, CO-pulse chemisorption revealed the quantitative synergistic effect between metal active sites and Brønsted acid sites. Catalysts with highly dispersed iron oxide and proper density of Brønsted acid sites exhibited the best catalytic performance. This study elucidated the catalytic roles of iron species and Brønsted acid sites in Fe/ZSM-5 catalysts in MDA and provided guidance for the future development of highly active MDA catalysts.
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高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Canyang Zhang,Guangtong Hai,Chao Chen,Yin Liang,Wei Zhao,Bolong Li,Jianghao Wang,Zhenyu Zhang,Huiping Ji,Kaige Wang,Reinout Meijboom,Jie Fu
The decarbonylation of biomass-derived fatty acids offers a green and sustainable route to high-value long-chain alkenes. Nitrogen-doped carbon-supported cobalt (Co-NC) catalysts have emerged as promising candidates for fatty acid decarbonylation, attributed to their exceptional catalytic activity and cost-effectiveness. However, identifying the active sites and elucidating the reaction mechanism remain significant challenges. To address these issues, we developed Co single-atom-rich catalysts (CoPc/MWCNT and pyrolyzed derivatives CoPc/MWCNT-X) via the impregnation of cobalt phthalocyanine onto multiwalled carbon nanotubes (MWCNTs), followed by pyrolysis. These catalysts exhibited a high stearic acid decarbonylation activity, increasing the heptadecene yield from 12.9 to 47.4%, with an alkene-to-alkane ratio of up to 4.3. Comprehensive characterization and control experiments conclusively demonstrated that Co single-atom sites serve as the active sites, while coexisting Co/CoO nanoparticles showed negligible activity and no synergistic effects. In situ DRIFTS revealed carbonyl group adsorption on Co single atoms, with DFT calculations confirming directional alkene production via C–O bond cleavage. This work establishes a facile synthetic strategy for high-performance decarbonylation catalysts and unambiguously identifies the critical single-atom active sites while enabling a profound understanding of fatty acid conversion mechanisms.
研究领域:
催化
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绿色化学
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材料科学
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化学反应工程
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表面化学
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DOI
高影响因子
Environmental Science-Nano
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2025
·
IF 5.1
Lu Wang,Siyuan Zhang,Jukun Xiong,Meicheng Wen
Formaldehyde (HCHO), a prevalent indoor volatile organic compound, poses significant health risks to humans even at very low concentrations. As a result, its efficient degradation at room temperature is of utmost importance. However, the detailed mechanism for catalytic oxidation of formaldehyde remains unclear, particularly regarding the role of water vapor, which has been subject to considerable debate. In this study, we synthesized Pt-supported TiO2 glass fiber catalysts (Pt/TiO2 GF) via NaBH4 reduction to investigate the reaction pathways and clarify the influence of water vapor on the oxidation process. The reaction mechanism and intermediates were systematically studied at room temperature using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), kinetic isotope effect (KIE) analysis, and density functional theory (DFT) calculations. Results revealed a clear reaction pathway of HCHO → DOM → HCOO− → CO2, with formate C–H bond cleavage (HCOO−* + O* → CO2 + OH*) identified as the rate-determining step. Both experimental KIE results and theoretical calculations confirmed that water vapor substantially reduces the activation barrier for this step, significantly promoting formate decomposition and subsequent CO2 formation. This work provides critical insights into the role of water in enhancing formaldehyde oxidation and offers theoretical support for developing efficient catalysts suitable for humid environments.
研究领域:
环境化学
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催化
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材料科学
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表面科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Baoxin Ni,Hua Jiang,WenYao Guo,Qunjie Xu,Yulin Min
The regulation and stabilization of the oxidation state to promote the conversion of CO 2 to C 2 fuel still faces many challenges. Based on the principle of charge balance, we creatively propose a co-doping strategy to adjust the surface oxidation state distribution of metallic catalysts . A TiO-based photocatalyst co-doped with Zn and N was synthesized by ammonia assisted one-step calcination method, named ZN-TC. XPS characterization shows that Zn and N adjust the valence states of adjacent Ti elements respectively, so that the surface of TiO maintains a relatively stable Ti 3+ /Ti 2+ ratio. Under visible light irradiation, the material can catalyze CO 2 into CO (324.11 μmol·g −1 ·h −1 ) and C 2 H 6 (10.27 μmol·g −1 ·h −1 ) in the liquid phase . The selectivity of C 2 H 6 reached 14.45%. When irradiated with near-infrared light, ZN-TC shows 100% CO selectivity because the photon energy is not enough to support the catalytic hydrogenation of CO 2 . Theoretical calculations and experiments proved that Zn and N elements mainly act on the B -1 band to regulate the Ti valence state. In-situ DRIFTS and in-situ Raman tests confirmed the function of oxidation state adjustment to promote the C-C coupling on the catalyst surface to produce ethoxy groups , which ultimately led to the production of C 2 H 6 .
研究领域:
材料科学
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环境科学
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化学工程
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物理化学
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纳米技术
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催化
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Le Yang,Rongrong Liu,Jun Liang,Li Li
The urgent need for sustainable carbon dioxide (CO 2 ) utilization has driven the development of photothermal catalysis as an efficient strategy for solar-driven CO 2 methanation. Herein, we report an amorphous nickel‑tungsten boride (NiWB) catalyst that achieves exceptional conversion of CO 2 to methane (CH 4 ) under mild conditions without external heating. The optimized NiWB catalyst exhibits a remarkable CH 4 production rate of 19.32 mmol g −1 h −1 with 92.50 % selectivity under full-spectrum illumination (2.0 W cm −2 ), surpassing most reported Ni-based catalysts. Structural and electronic characterizations reveal that the amorphous framework provides abundant unsaturated active sites, while W incorporation enhances interfacial interactions and modulates the electronic structure of Ni sites, promoting H 2 and CO 2 activation. In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFS) analysis confirms a formate-mediated reaction pathway, and kinetic studies demonstrate that photothermal synergy significantly reduces activation energy compared to pure thermal catalysis. Furthermore, the formation of stable W B bonds in amorphous catalyst inhibits crystallization, improving catalyst durability. This work highlights the synergistic advantages of amorphous engineering and electronic modulation in designing efficient photothermal catalysts for sustainable CO 2 valorization.
研究领域:
催化
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材料科学
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环境科学
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化学工程
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物理化学
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DOI
PubMed
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Jingxue Wang,Kang Sun,Denan Wang,Xinwei Niu,Zhongyuan Lin,Siyuan Wang,Weijie Yang,Jier Huang,Hai-Long Jiang
While the coordination environment around catalytic metal sites plays a crucial role in catalysis, its precise design and modulation still remain a challenge. Herein, the coordinated N atom number around single Co sites installed on a UiO-type metal–organic framework has been modulated to afford UiO-Co-Nx (x = 2, 3, and 4) for photocatalytic CO2 reduction. Significantly, the photocatalytic performance is affected by the coordinated N atom number around the Co site, in which UiO-Co-N3 exhibits superior activity to the other counterparts. Photo-/electrochemical results support the fastest charge transfer kinetics between the photosensitizer and UiO-Co-N3. Theoretical calculations, together with the results acquired from in situ diffuse reflectance infrared Fourier transform spectra, manifest the lowest energy barriers of the rate-determining step and desorption energy of CO* over UiO-Co-N3 among all UiO-Co-Nx samples.
研究领域:
化学
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材料科学
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催化
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环境科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Ziyi Zhang,Huiqing Dong,Dongxu Zhou,Kexin Tang,Yidi Ma,Tao Han,Jianqiu Lei,Shoushuang Huang,Xiaodong Zhang,Liang Tang,Ning Liu
Photocatalytic CO 2 reduction is a promising strategy to address both environmental issues and energy crisis. Defect engineering offers great potential for improving the photocatalytic performance. Herein, we report an innovative approach to introduce defects in MIL-68(In) via electron beam irradiation for the photoreduction of CO 2 into CH 4 . The irradiated X-MIL-68(In) (X mean the irradiation dose) retained the crystal structure and morphology of pristine MIL-68(In), while generating novel organic framework defects. These defects significantly improved the CO 2 photoreduction activity, with 300-MIL-68(In) achieving the highest CH 4 rate of 87.5 μmol g −1 h −1 and a CH 4 selectivity of 74.8 %. Comprehensive ex situ and in situ characterizations, combined with DFT calculations, demonstrated that defects formation in 300-MIL-68(In) accelerated the separation and transfer of photoexcited carriers, thereby driving its superior photocatalytic performance. Furthermore, In situ DRIFTS along with DFT calculations confirmed that ⁎ COOH, ⁎ CHO and ⁎ CH 2 O were key intermediates during CO 2 reduction process. This work highlights electron beam irradiation as an effective strategy for defect engineering, offering new opportunities for tuning the performance of photocatalysts.
研究领域:
材料科学
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环境科学
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纳米技术
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催化
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物理化学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Zhuangqing Wang,Xinchao Wang,Chao Zhang,Yinze Yang,Leilei Zhou,Haiyang Cheng,Fengyu Zhao
Catalytic conversion of furfural and its derivatives to value-added C 5 molecules has attractive much attention in the field of biomass conversion . In this paper, the selective hydrogenolysis of tetrahydrofurfuryl alcohol to 1,5-pentanediol has been studied over a series of PrO x promoted Ni/Al 2 O 3 catalysts. The catalytic performances and the promoting effects of PrO x , as well as the role of Ni and PrO x species have been discussed. The surface properties and structure of catalysts were examined by TEM, XRD, XPS, H 2 -TPR, H 2 -TPD, in-situ DRIFTS, etc. The presence of PrO x species promotes the reaction rate and changes product selectivity significantly, and a 79.2% 1,5-pentanediol selectivity can be obtained at 88.4% conversion over the NiPr 1.2 /Al 2 O 3 catalyst. The synergistic effect between defect-rich PrO x and the adjacent active Ni species has been confirmed to contribute to the superior catalytic performances. These results provide useful knowledge for the activation of cyclic ether bonds and the design of heterogeneous catalysts with lanthanide oxide supports.
研究领域:
催化
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生物质转化
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化学工程
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材料科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Qun Li,Tareque Odoom-Wubah,Yaping Zhou,Rafal Mulka,Yanmei Zheng,Jiale Huang,Daohua Sun,Qingbiao Li
The search for efficient and durable catalysts for volatile organic compounds oxidation is essential for environmental remediation. Herein, porous coral-like cobalt–manganese oxide (CoMnOx) catalyst was synthesized through annealing Co–Mn–1,3-propanediol precursors at 300 °C in air and applied for the catalytic oxidation of benzene. The as-prepared CoMnOx exhibited uniform porous coral-like structure, with an improved benzene catalytic abatement performance as compared to those of Mn3O4 and Co3O4 samples prepared by the same method, respectively. According to BET, H2-TPR, O2-TPD, and XPS analysis, the as-obtained CoMnOx catalyst showed the highest BET surface area, better low-reducibility temperature, and high content of absorbed oxygen groups when compared to Mn3O4 and Co3O4, which makes significant contribution to its catalytic benzene oxidation activity. Moreover, a plausible surface reaction mechanism for benzene oxidation over CoMnOx catalyst was also proposed through the in situ DRIFTS study.
研究领域:
环境科学
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催化
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材料科学
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高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 20
·5098-5107
·
IF 4.495
Ning Xiang,Yaqin Hou,Xiaojin Han,Yulin Li,Yaoping Guo,Yongjin Liu,Zhanggen Huang
Room temperature HCHO catalytic oxidation over inert support loaded Pd catalysts remains a significant challenge. Herein, a series of alkali Na (1–4 wt.%) modified 1Pd/SBA-15 catalysts were prepared by a co-impregnation method and used for HCHO catalytic oxidation at room temperature. Results showed that alkali Na significantly improved the HCHO oxidation performance of 1Pd/SBA-15 and the optimal Na loading was 2 wt.%. BET, XRD, STEM, XPS, H 2 -TPR, O 2 -TPD and in situ DRIFTS were performed to reveal the promotion role of alkali Na. As a consequence, alkali Na addition could stabilize well dispersed Pd particles which then facilitated the O 2 activation and accelerated the decomposition of formate intermediates species, thus a superior HCHO catalytic oxidation performance was obtained. This study first clearly illustrated the promotion mechanism of alkali Na without the implication of active support and provides an efficient and facile way to achieve high dispersion of Pd particles on inert support and tremendously expands the selected range of supports for room temperature HCHO catalytic oxidation. Graphical Alkali promoted : A series of Na alkali-promoted 1Pd/SBA15 catalysts were prepared by a co-impregnation method and tested for HCHO catalytic oxidation at room temperature. Addition of alkali Na stabilized well-dispersed Pd particles which facilitated O 2 activation and accelerated formate species decomposition rate, leading to superior HCHO catalytic oxidation performance of 2Na-1Pd/SBA-15.
研究领域:
催化化学
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环境科学
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材料化学
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表面科学
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大气污染控制
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DOI
高影响因子
BIOMASS & BIOENERGY
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2024
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IF 5.8
Yong Liu,Jirong Long,Zhijiao Huang,Lungang Chen,Chenguang Wang,Xinghua Zhang,Longlong Ma
Direct production of 2,5-dimethylfuran (DMF) from fructose is crucial for developing biomass-derived fuels, yet it presents significant challenges due to the need for multifunctional active sites for dehydration and hydrodeoxygenation. Meanwhile, the disposal of wine lees, a major winemaking by-product, incurs substantial costs. Herein, a hybrid catalyst system of sulfonated wine lees carbon (WLC-SO 3 H) and PtFe/C was introduced, achieving a DMF yield of 66.4 % directly from fructose. WLC-SO 3 H, with enhanced Brønsted acidity, demonstrated high activity in dehydrating fructose to 5-hydroxymethylfurfural (HMF) with a 98.2 % yield. PtFe/C effectively catalyzed the hydrodeoxygenation of HMF to DMF, driven by the strong interaction between Pt and Fe species. This interaction was confirmed through in situ DRIFTS and theoretical calculations, highlighting the system's superior catalytic performance.
研究领域:
化学工程
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催化
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可再生能源
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生物质转化
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Qiuhui Zhu,Reshalaiti Hailili,Yue Xin,Yingtang Zhou,Yu Huang,Xinzhu Pang,Ke Zhang,Peter K.J. Robertson,Detlef W. Bahnemann,Chuanyi Wang
Developing full-spectrum responsive and efficient photocatalysts is still an important challenge in the field of photocatalytic treatment of trace environmental pollutants. Herein, full-spectrum Bi@Bi 2 Ti 2 O 7 with rich-oxygen vacancies (OVs) were fabricated via a one-pot hydrothermal method. The optimized composite photocatalyst exhibited a photocatalytic efficiency of 79 %, more than doubled higher than that of its counterpart, Bi 2 Ti 2 O 7 (31.79 %), for removing ppb-level NO under visible-near infrared (Vis-NIR) irradiation. The enhanced photocatalytic performance was attributed to the co-effect of Bi and OVs reveal by control experiments and theoretical calculations, which not only benefited the adsorption and photocatalytic activation of NO but broadened light absorption to near infrared region. Furthermore, the adsorption and photocatalytic conversion pathway of NO was explored by in situ DRIFTS, suggesting that NO + as intermediate species is crucial to improve the selectivity of NO converting to nitrate. This work provides a new perspective of constructing full-spectrum-driven photocatalysts for environment remediation.
研究领域:
环境科学
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材料科学
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光催化
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DOI
高影响因子
危险品化学品经营许可证（带存储）