APPLIED CATALYSIS A-GENERAL
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2019
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IF 4.63
Shiqiu Zhang,Xue Yang,Kui Zheng,Ruihao Xiao,Qidong Hou,Bangjun Liu,Meiting Ju,Le Liu
It is a promising pathway to reduce the dependence on fossil fuels and obtain the bio-fuels or chemicals production from biomass derivatives. The conversion from furfural (FFR) to furfuryl alcohol (FFA) is an important industrial technology using the liquid-phase hydrogenation method with external hydrogen gas. However, the natural environment is threatened by the security of external hydrogen gas, toxicant catalyst, and the high energy consumption. Recently, in-situ hydrogenation is a novel method to converse FFR to FFA at mild reaction conditions to replace the dangerous external hydrogen gas. In this paper, we reported an efficient in-situ hydrogenation method via aqueous-phase reforming of methanol using Pt loading MgTiO 3 (perovskite-type material) at mild conditions. Pt nanoparticles were high dispersion on the nano-MgTiO 3 -450 surface, and CH 3 OH and H 2 O were reformed to produce hydrogen gas on the catalyst surface through the action of Pt nanoparticles. A part of active hydrogen could be involved in the reduction of Pt 2+ to Pt 0 , resulting in the perfect recyclability of the Pt@MT-450 catalyst. The other part of active hydrogen were participated in the hydrogenation of FFR conversion to FFA under the interaction of Pt and Mg elements. The in-situ hydrogenation of FFR to FFA using Pt@MT-450 is an effectively pathway to reduce the reaction conditions than that with external hydrogen gas.
研究领域:
能源化学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Jinrong Liang,Kejia Wu,Fukun Li,Jinxing Long,Qiang Zeng,Xuehui Li
Catalytic hydrogenolysis of the renewable aromatic polymer of lignin to value-added fine chemicals without external molecular hydrogen is of great significance. In this work, catalytic conversion of lignin with in situ H 2 produced from the aqueous phase reforming (APR) of methanol is studied in the presence of ZnO-modified Pd/AC (Pd-Zn/AC). 259.8 mg g -1 yield of monophenols is obtained when the lignin depolymerization is catalyzed by Pd-Zn/AC-10 in a methanol aqueous solution ( V C H 3 OH / V H 2 O =9/1) at 250 °C for 4 h. Extensive analysis showed that this effective process should be attributed to the synergistic effect between Pd-Zn alloy and the metallic Pd, which promote the H 2 production from the APR of methanol and the hydrogenolysis of lignin, respectively. Moreover, a plausible pathway for selective hydrogenolysis of lignin is proposed based on the comparative characterization of the raw lignin, residual lignin, and the transformation behavior of lignin model compounds.
研究领域:
化学工程
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可再生资源化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Jiajin Li,Minglei Lu,Yuxin Ge,Weiwei Lu,Zidi Liu,Hongde Xu,Yu Zhang,Zhihui Li,Zhuoyu Zheng,Pengxiang Gao,Qian Zhang,Tiejun Wang
Aqueous-phase reforming of methanol (APRM) is an important method for H 2 production, widely used in energy fields like polymer electrolyte membrane fuel cells (PEMFCs). However, traditional noble metal catalysts , being expensive and vulnerable to CO poisoning, restrict their practical application. Therefore, developing robust non-noble metal catalysts for efficient and sustainable H 2 production with low CO levels in APRM at low temperatures is highly significant. In this study, a novel approach was employed to synthesize carbon-encapsulated Cu catalyst via controlled pyrolysis , leading to Cu@CA-Val catalyst with excellent low-temperature catalytic activity. The optimal Cu@CA-Val-300 catalyst exhibited a high hydrogen production rate of 0.2–27.0 μmolH 2 /g cat /s over a wide temperature of 135–180 °C (base-free), surpassing the most Cu-based and Pt-based catalysts. The Cu@CA-Val-300 catalyst exhibited exceptional hydrothermal stability during continuous operation in a fixed reactor for 200 h. Efficient H 2 production was attributed to good wettability , enabling the diffusion of CH 3 OH and H 2 O molecules into Cu + /Cu 0 sites for activation, with CO being suppressed and transformed through the formate formation.
研究领域:
能源化学
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
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2019
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IF 12.221
Didi Li,Yi Li,Xiaohui Liu,Yong Guo,Chih-Wen Pao,Jeng-Lung Chen,Yongfeng Hu,Yanqin Wang
The production of hydrogen from the aqueous-phase reforming (APR) of oxygenated hydrocarbons is promising. Herein, the performances of Pt loaded on NiAl2O4 spinel and γ-Al2O3 were investigated in the APR of methanol. The conversion of methanol and the yield of hydrogen over Pt/NiAl2O4 reached 99.9% and 95.7%, respectively. In comparison with Pt/γ-Al2O3 catalyst (26.5% and 23.3%, respectively), these values were enhanced by 4-fold. More importantly, Pt/NiAl2O4 had high stability with only 10% loss of its initial conversion after 600 h on stream. In situ diffuse reflectance infrared Fourier transform spectra (DRIFTS) of the APR of methanol revealed that the reaction underwent the dehydrogenation of methanol and the sequential water–gas shift (WGS) reaction. These two reactions were then investigated independently, in which Pt/NiAl2O4 showed more efficient performance than Pt/γ-Al2O3. Intensive characterization methods revealed that the chemical state of Pt played a pivotal role in the dehydrogenation of methanol to generate the adsorbed CO intermediate. For Pt/NiAl2O4 catalyst, the reduction of PtOx to metallic state Pt was easier because of the presence of the oxygen vacancy, leading to the higher catalytic performance in the dehydrogenation of methanol. Further studies with in situ DRIFTS-MS of WGS demonstrated a redox mechanism over Pt/NiAl2O4 catalyst, which was different from the associative route that occurred over Pt/γ-Al2O3 and made the WGS reaction faster. The addition of Ni (NiAl2O4 spinel) creates oxygen vacancies, giving WGS which underwent a redox route. This work presents the deep understanding into the pathway and mechanism in the APR of methanol and is expected to have important implications for the future development of APR catalysts.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
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2017
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IF 3.833
Rui Chen,Ning Ren,Xin Jin,Xinyuan Zhu
Poly(N-isopropylacrylamide) (PNIPAM)-based ionic microgels with different diameters were first prepared and then used as particulate stabilizer or seed in dispersion polymerization of styrene. The role of PNIPAM-based ionic microgels could be transformed from particulate stabilizer to seed by controlling the water content in methanol–water mixture. Generally, PNIPAM-based ionic microgels served as particulate stabilizer in methanol in the absence of water, leading to the formation of spherical polystyrene nanoparticles. However, they turned into seeds when water was added into the methanol solution, with the formation of octopus-like nanoparticles. Further study demonstrated that the mechanism for this role transition was related to the special thermosensitivity of PNIPAM microgels in methanol–water mixture. They lost their thermosensitivity in pure methanol solution but restored their thermosensitivity when increasing the water content in methanol–water mixture.
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
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Zhongming Hao,Xinghong Duo
Enhancing photocatalytic performance relies on efficient and stable solar energy utilization, broadening visible light absorption, and optimizing interfacial charge transfer mechanisms. We successfully synthesized lead-cerium co-doped TiO2 enriched with oxygen vacancies (Tiδ+-Ov(-Ceδ+)-Pb2+) using sol-gel and direct addition methods. Results show that Pb2+ ions are uniformly distributed within the oxygen vacancy-rich TiO2 lattice, synergizing with surface-embedded Ce2+/Ce3+ ions to extend the visible light absorption range of TiO2. This led to a 32.3% increase in light absorption and an approximate 90% improvement in photoelectric conversion efficiency. The maximum photocurrent density reached 3.1 μA/cm², with a reduction of 0.15 eV in the initial oxidation potential and a 30% decrease in bandgap width. Under simulated sunlight (AM1.5G), the hydrogen production rate of Tiδ+-Ov(-Ceδ+)-Pb2+ was 11.516 μmol/h/g, double the combined output of TiO2-Ce and TiO2-Pb. Mechanistic analysis reveals that the superior performance stems from the interfacial sites in Tiδ+-Ov(-Ceδ+)-Pb2+, where the low-valent Pb2+ and variable-valent Ce3+/Ce4+ ions act as charge traps that promote efficient charge separation. Furthermore, surface-embedded Ce generates an uneven surface potential, facilitating the adsorption of formaldehyde molecules from the solution onto the modified TiO2 surface and improving carrier dynamics. These findings provide new strategies for designing and optimizing high-efficiency photocatalytic materials.
研究领域:
材料科学
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能源科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2024
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IF 6.7
Baozhu Chen,Zefeng Zheng,Changsong Hu,Ziyu Zengcai,Zhonghai Liu,Minglei Lu,Qingwei Meng,Tiejun Wang
The development of a highly efficient non-noble catalyst for rapid releasing of hydrogen from methanol/water at low temperature is urgent, but challenge. In this paper, the high content of graphited N-doped carbon encapsulated reducing state copper catalyst was fabricated for low-temperature aqueous reforming of methanol. The Cu@NGC-600 catalyst gives excellent hydrogen production rate of 46.15 μmol·g cat -1 ·s -1 at 190 °C, which is 4 times higher than the commercial 20 % Pt/C catalyst and 3 times higher than other reported Cu-based catalysts (such as the Cu@NC-200 catalyst). Characterization and DFT calculation results revealed that rich doping of graphite N and the synergistic effect of Cu–N strengthened the electron transfer between copper and the NC matrix, decrease the reduction temperature of catalyst, which enabled the Cu to maintain a highly reduced state of Cu 0 /Cu + during APRM for low temperature (150–190 °C) hydrogen production.
研究领域:
化学工程
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催化材料
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Yuyao Yang,Xuan Bie,Xiaoying Qi,Yongqing Xu,Qinghai Li,Yanguo Zhang,Hui Zhou
Aqueous phase reforming of methanol (APRM) offers a method for releasing H2 from the liquid phase, by which H2 can be stored in methanol safely. It is an efficient way to design high-performance catalysts by controlling the hydroxyl (OH) groups, but its mechanism for affecting the APRM is still unclear. Herein, we loaded Pt on three types of Al2O3 (nanopolyhedron, nanosheet, and nanorod Al2O3) with different OH contents and types. Among them, Pt/nanorod Al2O3 exhibited the highest H2 production rate of 20.4 μmol g–1 s–1 with 96.6% H2 selectivity at a low temperature of 190 °C. This was attributed to the roles of hydroxyl groups in modulating Pt states. On nanopolyhedron, nanosheet, and nanorod Al2O3, the bonding of Pt with O atoms became more favorable as the dehydroxylation happened. In particular, on nanorod Al2O3, the dehydroxylation process generated a high density of five-coordinated Al (AlV) sites, facilitating the dispersion and anchoring of Pt particles. Moreover, the special OH groups (hydrogen bond donor) on nanorod Al2O3 promoted Pt particle reduction via the movement of electrons. Ultimately, the results demonstrated the influence of OH groups on the dispersion and reduction of active metals, offering perspectives for designing catalysts for APRM through hydroxyl control.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Jianxian Li,Wenting Lin,Minglei Lu,Junwei Liao,Changsong Hu,Tiejun Wang
Efficient release of H 2 with negligible CO impurities from sustainable MeOH/H 2 O has become a promising goal for on-board hydrogen generator. However, hydrogen release kinetics still face challenges. In this work, the Cu/ZnO/CeO 2 catalyst with high density ultra-small Cu nanoparticles and abundant oxygen vacancies were prepared for intensifying hydrogen evolution in aqueous phase reforming of methanol (APRM). The optimized 55% Cu/ZnO/CeO 2 catalyst (Cu NPs of 3.8 nm, Cu loading of 55.89 wt%, oxygen vacancies of 2.316 × 10 15 spins g −1 ) exhibited an excellent H 2 evolution rate of 58.39 μmolg cat −1 s −1 even at low temperature of 210 °C, which was 2.1-fold enhancement than that of commercial Cu/ZnO/Al 2 O 3 catalyst. Characterizations and experiments revealed that ZnO/CeO 2 intensified the strong metal-support interaction (SMSI), which anchored the Cu NPs, generated abundant oxygen vacancies and adjusted electronic structure to form Cu 0 -Cu + -O v active sites for facilitating the kinetics of APRM.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Haiping Zhu,Yuxin Ge,Pengcheng Zhao,Zihan Sun,Zhuoyu Zheng,Fan Yang,Lin Chen,Yongqi Mao,Xueer Huang,Jiajin Li,Minglei Lu,Tiejun Wang
Aqueous phase reforming of methanol (APRM) is a promising technology for efficiently producing hydrogen (H 2 ) in a sustainable approach, enabling convenient and safe H 2 storage and transportation. Herein, we develop a Ni/Cu/Cu 2 O@CA catalyst with excellent performance by integrating density functional theory (DFT) calculation and experimental investigations. DFT results show that Ni doping greatly reduced the activation energy (E a ) of CH 3 OH dehydrogenation and H 2 O dissociation, especially the E a of the rate-limiting step of CH 3 O∗ → CH 2 O∗ + H∗ from 1.71 eV to 1.28 eV. Additionally, the Cu/Cu 2 O(111) surface is found to promote the CO conversion. To verify the synergistic effect between Ni and Cu/Cu 2 O(111), a 3D spherical porous Ni/Cu/Cu 2 O@CA catalyst is synthesized for APRM experiments, achieving a peak H 2 production rate of 135.93 μmolH 2 /g cat /s at 240 °C, which is 2.0 times higher than that of the Cu/Cu 2 O@CA catalyst. Overall, this work presents an implementable strategy for developing non-noble metal catalysts for sustainable H 2 production.
研究领域:
催化化学
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
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2025
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IF 17.1
Zhao Sun,Huicai Wang,Xingxu Wang,Riguang Zhang,Zhiqiang Sun
Sorption-enhanced steam reforming of methanol (SE-SRM) offers a promising route for high-quality hydrogen production with in situ CO 2 capture; however, achieving an optimal balance between catalytic activity and CO 2 uptake capability, while ensuring catalyst stability, remains a significant challenge. In this study, a series of Zr-doped (0 wt%, 5 wt%, 15 wt%, 25 wt%) Cu-MgO catalytic sorbents are synthesized for SE-SRM. At 180℃, the hydrogen concentration and yield reach nearly 100 % and 10.35 μmol·g −1 ·s −1 . Moreover, the catalytic sorbent basically retains its catalytic activity and CO 2 uptake capacity after 30 cycles with merely slight deactivation. Results demonstrate that the doped Zr, presents as tetragonal ZrO 2 , enhances metal-support interactions with the formation of a Cu-O-Zr interfacial structure, promoting Cu nanocluster dispersion and altering the Cu + /Cu 0 distributions. Zr doping also enables the modulation of the medium-strong basic sites. Moreover, the AFM and TEM confirmed the formation of high-roughness MgO surface on the substrate, thereby facilitating CO 2 diffusion and adsorption. DFT calculation results further confirm the advantages of Zr-doped Cu-MgO catalytic sorbents due to its stronger capability on CH 3 OH activation and CO 2 adsorption.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Qiuwan Shen,Zhongwen Cai,Xin Zhang,Gaokui Chen,Guogang Yang,Shian Li
A series of CuFe x Al 2−x O 4 (0
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）