JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 99
·期 4
·922-930
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IF 2.8
Dingshuo Zhang,Heqian Zhang,Yue Li,Daolai Sun,Jianhua Lv
BACKGROUND Levulinic acid is an important platform chemical derivable from lignocellulosic biomass. In this work, the hydrogenolysis of levulinic acid to produce 1,4-pentanediol was performed over some Co-based non-noble catalysts. The relationship between the catalyst properties and the catalytic activity was investigated, and the effects of the reaction conditions on the catalytic activity were studied. RESULTS The Co/ZrO 2 catalyst prepared by a coprecipitation method showed a high catalytic performance in the hydrogenolysis of levulinic acid to form 1,4-pentanediol. The calcination of Co/ZrO 2 significantly affected the catalytic activity, and a high calcination temperature of 750 °C could promote the formation of 1,4-pentanediol. Meanwhile, the reduction of Co/ZrO 2 at 400 °C in an H 2 flow was beneficial for producing 1,4-pentanediol, and the Co species after the reduction existed as the forms of Co 2+ and Co 0 . A high H 2 pressure and a moderate reaction temperature of 200 °C were beneficial for producing 1,4-pentanediol, and a high 1,4-pentanediol selectivity of 85.6% with a complete conversion of levulinic acid was obtained over the Co/ZrO 2 catalyst at 200 °C under an H 2 pressure of 7 MPa. CONCLUSION The Co species in the 400 °C-reduced Co/ZrO 2 catalyst existed as the forms of Co 2+ and Co 0 . It was proposed that the synergistic effect of Co 2+ and Co 0 contributed to the effective formation of 1,4-pentanediol from levulinic acid. © 2024 Society of Chemical Industry (SCI).
研究领域:
化学工程
·
可再生能源
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Jiaojiao Tan,Jiaming Wang,Ziyang Zhang,Zhi Ma,Luhui Wang,Yuan Liu
To improve the catalytic activity of CO 2 methanation at low temperature, a series of Ni/ZrO 2 catalysts with different Ni loadings were prepared by citrate complexing method. Based on the optimal Ni loading of 6 wt%, a certain amount of MgO was doped to improve the thermal stability of Ni/ZrO 2 catalyst. When Ni/Mg molar ratio was 4, there was the best performance, getting as high as 90% CO 2 conversion and nearly 100% CH 4 selectivity at 250 °C, 0.1 MPa and a WHSV of 15,000 ml g −1 h −1 , and the equilibrium CO 2 conversion was obtained at 300 °C. XRD , BET, TPR, CO 2 -TPD, H 2 -TPD, XPS , TG and TEM were conducted to investigate the reason of high activity of Ni/ZrO 2 catalyst at low temperature and the effect of doping MgO. Results suggested that highly dispersed Ni nanoparticles are responsible for the excellent catalytic activity. MgO can effectively improve stability of Ni-based catalysts by the confinement effect. Meanwhile, it is also found that there are little improvements on catalytic activity after doping MgO, and the TOF of catalysts with different MgO doping is basically the same, indicating CO 2 can be efficiently adsorbed and activated on the monoclinic ZrO 2 , and MgO do not contribute to the intrinsic activity.
研究领域:
催化
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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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fan Xu,Xin Meng,Rui Zhao,Daoming Jin,Wenhua Dai,Dandan Yang,Zhong Xin
The utilization of CO 2 for the production of light olefins through catalysis with iron-based catalysts presents a viable strategy to address the challenges of carbon neutrality. In this study, we synthesized a novel hybrid catalyst Fe 2 O 3 @ZrO 2 , derived from the pyrolysis of dual metal–organic frameworks (NH 2 -MIL-88B@UiO-66). Under specific conditions (340 °C, 3.0 MPa, CO 2 /H 2 = 1:3, 10000 mL g cat −1 h −1 ), the Fe 2 O 3 @ZrO 2 catalyst exhibited a notable space–time yield of light olefins at 12.7 mmol g −1 h −1 . The characterizations results show an electron transfer from ZrO 2 to the Fe 2 O 3 surface was observed at the heterointerface of Fe 2 O 3 and ZrO 2 . This electron transfer mechanism was identified as advantageous for the formation of the active phase Fe 5 C 2 . This research introduces an innovative use of the hybrid Fe 2 O 3 @ZrO 2 catalyst derived from MOF-on-MOF, holding significant promise in advancing the field of CO 2 hydrogenation catalysts.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2015
·
IF 2.605
Meng Zhao,Xiaorui Ren,Jun Yang,Wei Pan
A series of ThO 2 -doped Y 2 O 3 stabilized ZrO 2 monolith compounds were prepared and investigated. The bigger ionic radius of Th 4+ substitutions dilutes the average oxygen coordination to the cations, which is the determinant factor of the phase stability. Therefore, ThO 2 incorporation has a strong impact on the phase composition, and consequently on the thermo-mechanical properties of the specimens. The metastable t′ phase was stabilized in light-doped specimens with a decreasing tetragonality while the thermodynamic equilibrium t phase and the related martensitic t–m phase transformation were absent in ThO 2 -doped specimens. Additionally, lower thermal conductivity was also achieved due to the substitutional phonon scattering effect. Considering the phase stability and thermo-mechanical properties, ThO 2 -doped Y 2 O 3 stabilized ZrO 2 compounds may be promising candidates for thermal barrier coatings although further research may be needed to improve their mechanical properties.
研究领域:
材料科学
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热物理
✓ 已验证
DOI
高影响因子
ADVANCED ENGINEERING MATERIALS
·
2022
·Vol. 24
·期 8
·2101603
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IF 4.122
Jianhong Dong,Yongshuai Xie,Lixin Liu,Zhezhe Deng,Wei Liu,Luyi Zhu,Xinqiang Wang,Dong Xu,Guanghui Zhang
Low density, heat-resistant sponge-like fiber assembly materials are considered as promising high-temperature insulation materials. However, the poor structural stability, infrared radiation heat transfer, and complex preparation process limit its further application. Herein, a facile method to create ultralow-density ZrO 2 –TiO 2 fiber sponges by the electrospinning method followed by heat treatment is presented. The layered structure sponges treated at 1200 °C have a low density of 9.5 mg cm −3 . Moreover, the sponges possess high compressibility and good compression resistance over a wide temperature range from −196 to 1200 °C. In addition, the sponges exhibit low thermal conductivity of 27 mW m −1 K −1 , robust fire resistance, and high near-infrared reflectance, making them an ideal alternative for high-temperature thermal insulation materials.
研究领域:
材料科学
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Nana Gong,Tao Zhang,Minghui Tan,Liyan Wang,Jiaqian Yang,Li Tan,Guohui Yang,Peng Wu,Yingquan Wu,Yisheng Tan
CO hydrogenation to isobutyl alcohol is a promising route for CO transformation to high value-added products. However, the formation mechanism of isobutyl alcohol is complex, and its synthesis requires complex catalysts and harsh reaction conditions, which hinders the identification of active sites. Herein, we efficiently synthesized isobutyl alcohol under mild conditions over a simple Cu–ZrO2 catalyst by decreasing the Cu loading. The space–time yield (STY) of isobutyl alcohol using an optimal CZ-0.11 catalyst was as high as 61.3 g·Lcat–1·h–1 with a CO conversion of 19.2%, far surpassing the STY of the state-of-the-art isobutyl alcohol synthesis (44.6 g·Lcat–1·h–1) under harsh conditions. Decreasing the Cu loading increased the distribution of smaller Cu particles and clarified the structure–activity relationship of Cu–Zr interactions for isobutyl alcohol synthesis. The enhanced Cu–Zr interaction led to the formation of more electron-deficient Cu species on the CZ-0.11 catalyst, which enriched the linearly adsorbed CO on Cu, as demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy. Experimental and theoretical results revealed that coupling of the bicarbonate species on ZrO2 with the linearly adsorbed CO species on electron-deficient Cu clusters promoted the formation of C2 intermediates and finally produced isobutyl alcohol through rapid β-addition. These insights into the active sites for CO hydrogenation to isobutyl alcohol may guide further catalyst designs.
研究领域:
催化化学
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能源化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7268-7277
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IF 6.119
Weixiao Sun,Peng Lin,Qinghu Tang,Fangli Jing,Qiue Cao,Wenhao Fang
The synergistic effect between bimetallic nanoparticles, as well as the support effect, is particularly important for supported catalysts in heterogeneous catalysis. In this work, an AgPd/ZrO2 bimetallic catalyst was reported for the base-free aerobic oxidation of vanillyl alcohol to vanillin, a challenging transformation of an aromatic bio-alcohol into a valuable fine chemical. The crystalline structure and textural properties of ZrO2 were modulated by using different zirconium precursors and precipitants during the precipitation process. The ZrO2 obtained from zirconium nitrate and trimethylamine was found to be the most suitable support. It displayed abundant reactive oxygen species and the largest specific surface area. Then, an Ag promoter was added to the Pd/ZrO2 catalyst and the synergy between Ag and Pd was tuned by varying their ratios. The Ag0.5Pd1/ZrO2 catalyst showed an enhanced performance, i.e., 100% conversion of vanillyl alcohol and 95% selectivity to vanillin at 120 °C and 3 bar O2 within 4 h, in comparison with the Pd/ZrO2 catalyst (69% and 87%, respectively). Moreover, the vanillin productivity reached 133.0 mol mol−1 h−1, the best result reported in the literature to date. Various characterization methods demonstrated that the addition of Ag can reduce the mean size of Pd nanoparticles (4.9 nm vs. 3.8 nm), and Ag+ species were beneficial to stabilizing Pd0 species in a high fraction due to electron transfer. The reactive Pd0 sites closely interacting with the Ag promoter allowed lowering of the apparent activation energy of the reaction (27.3 vs. 37.5 kJ mol−1). In addition, the Ag0.5Pd1/ZrO2 catalyst exhibited superior stability during consecutive recycling uses owing to the strong metal–support interactions.
研究领域:
催化化学
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材料科学
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绿色化学
✓ 已验证
DOI
高影响因子
Desalination and Water Treatment
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2024
·
IF 1
Jing Yang,Siyuan Yang,Jing Zhang,Jian He,Wei Jiang
ABSTRACT The recovery of Cr(VI) from the solution and the utilization of by-products are significant for waste-water treatment and environmental protection. In this study, the amorphous ZrO 2 was prepared using a solvothermal method and used to treat the wastewater containing Cr(VI). Amorphous ZrO 2 is effective for the photocatalytic reduction of Cr(VI). Without a sacrificial agent, 20 mL potassium dichromate solution (20 mg/L) is reduced to almost 0 mg/L within 10 min. Moreover, the by-products obtained from this process exhibit good performance in the catalytic dehydrogenation of ethane coupled with the reverse water–gas reaction. The maximum yield of ethylene is 12.9%, and the service life of the catalyst reached 160 min. Catalyst deactivation is caused by carbon deposition, and the deactivated catalyst is regenerated by roasting in the air. The feasibility of this green process is demonstrated, including the one-step photocatalytic reduction of Cr(VI) and utilization of the by-product as an ethane dehydrogenation catalyst.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
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2016
·Vol. 11
·期 24
·3541-3549
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IF 4.592
Xin Zhang,Ruyan Wu,Zeyi Wang,Mingxia Gao,Hongge Pan,Yongfeng Liu
Graphical Boosting hydrogen storage : In situ-synthesized nanocrystalline ZrO 2 @C exhibits good catalytic activity for hydrogen storage in NaAlH 4 . The NaAlH 4 –7 wt % ZrO 2 @C sample releases hydrogen starting from 126 °C and reabsorbs hydrogen starting from 54 °C, and these temperatures are lower by 71 and 36 °C, respectively, than those for pristine NaAlH 4 (see figure). Sodium alanate (NaAlH 4 ) has attracted intense interest as a prototypical high-density hydrogen-storage material. However, poor reversibility and slow kinetics limit its practical applications. Herein, a nanocrystalline ZrO 2 @C catalyst was synthesized by using Uio-66(Zr) as a precursor and furfuryl alcohol (FA) as a carbon source. The as-synthesized ZrO 2 @C exhibits good catalytic activity for the dehydrogenation and hydrogenation of NaAlH 4 . The NaAlH 4 -7 wt % ZrO 2 @C sample released hydrogen starting from 126 °C and reabsorbed it starting from 54 °C, and these temperatures are lower by 71 and 36 °C, respectively, relative to pristine NaAlH 4 . At 160 °C, approximately 5.0 wt % of hydrogen was released from the NaAlH 4 -7 wt % ZrO 2 @C sample within 250 min, and the dehydrogenation product reabsorbed approximately 4.9 wt % within 35 min at 140 °C and 100 bar of hydrogen. The catalytic function of the Zr-based active species is believed to contribute to the significantly reduced operating temperatures and enhanced kinetics.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Pengsen Zhao,Haizhong Zheng,Guifa Li,Yongxiang Geng,Yixin Xiao,Hongbo Guo,Ping Peng
The CaO–MgO–Al 2 O 3 –SiO 2 (CMAS) corrosion resistance of La 3+ -Yb 3+ -Ce 4+ co-doped ZrO 2 (LYZC) ceramic was systematically discussed via experiment and first-principles calculation. Results demonstrate that at the CMAS/RE-ZrO 2 interface, RE is dissolved in molten CMAS to form some RE-apatite particles, which effectively inhibits CMAS penetration. Compared with La 3+ doped ZrO 2 (LZ), LYZC owns a better ability to maintain the coating microstructure under CMAS corroded, which is conducive to alleviating CMAS penetration. This conclusion is also confirmed by the low diffusion coefficients ( D ) of RE and Zr in CMAS/LYZC(111), which are only 2.305–5.556 × 10 −8 m/s and 2.694–3.421 × 10 −8 m/s, respectively. Furthermore, the small electrostatic potential difference (Δ V = 1.578–1.654 eV) of the CMAS/LYZC(111) terminal layer suggests that molten CMAS does not easily adhere to the LYZC surface.
研究领域:
材料科学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Yujuan Jing,Pingquan Wang,Qiangbin Yang,Qiurun Wang,Yang Bai
Faced with severe corrosion of casing in oil wells, the epoxy coating was applied to prevent corrosion. Based on the mechanism that the filler eliminated the internal stress during the curing process of the coating and prevented the penetration of corrosive medium into the coating, a new filler was successfully prepared by the hydrothermal method . When the molar ratio of the precursor of ZrO 2 to MoS 2 was 1.2:1, MoS 2 was uniformly modified with ZrO 2 through mussel inspired chemistry of dopamine. Introducing fillers into epoxy coatings, specifically, a proper content of 0.8 wt.% filler can greatly improve the mechanical properties and corrosion resistance of the coatings. The coating maintained the excellent corrosion resistance for 16 h under high temperature (108 °C) and high pressure (pressurized with CO 2 gas of 35 MPa), which would provide us a reliable anticorrosive coating for oil wells metal casing.
研究领域:
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 Materials Chemistry C
·
2020
·Vol. 8
·期 13
·4518-4533
·
IF 7.059
Guo-Hui Pan,Liangliang Zhang,Huajun Wu,Xuesong Qu,Hao Wu,Zhendong Hao,Ligong Zhang,Xia Zhang,Jiahua Zhang
Monoclinic ZrO2 (m-ZrO2) is an attractive material for photonic applications due to its low site symmetry and phonon energy. In this paper, we present detailed studies on the luminescence properties of Ti4+ and Eu3+ in m-ZrO2. In view of the continuing controversy over the origin of “intrinsic” white-blue luminescence in pristine m-ZrO2, more spectroscopic information obtained by characterizing m-ZrO2 intentionally doped with Ti4+, Ti3+ and other metal ions and extensive discussions on the general characteristics of different luminescence processes were provided to evidence the luminescence as the Ti3+ → O− charge transfer transition in the [Ti(IV)O7]10− complex due to the trace amount of Ti4+ impurity in ZrO2 reagent. Competitive absorption was observed between host exciton and oxygen–metal charge transfer processes (O2−–Ti4+, O2−–Eu3+), and even between the two types of charge transfer process because of the sharing of electrons at the top of the valence band, which greatly influenced the absorption and excitation processes. The spectral components comprising the broad excitation band of O2−–Ti4+ white-blue or Eu3+ red emissions in different phosphors were identified, and their evolutions with doping concentration were explained. The energy state locations of oxygen defects produced by intrinsic charge compensation in m-ZrO2:Eu3+ were proposed to be ∼2.41 eV above the top of the valence band by using Eu3+ for the luminescent probe. Efficient energy transfer from the [Ti(IV)O7]10− complex to Eu3+ was first observed in m-ZrO2:Ti4+,Eu3+ phosphors, which were demonstrated to be high performance ratiometric self-referencing optical thermometric materials based on the dual-emitting combination strategy, with the relative sensitivity amounting to ∼3.84% K−1. Optical thermometry not only covering the physiological temperature range but also with high relative sensitivity could be achieved upon appropriate doping.
研究领域:
材料科学
·
光物理学
✓ 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）