CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Junbo Feng,Junyan Wu,Dongdong Yan,Yadong Zhang
Porous silica nano-flowers (KCC-1) immobilized Pt-Pd alloy NPs (Pt-Pd/KCC-1) with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction, using hydrazinium hydroxide as a reducing agent. The as-synthesized silica nanospheres possess radial fibers with a distance of 15nm, exhibiting a high specific surface area (443.56 m 2 ·g –1 ). Meanwhile, the obtained Pt-Pd alloy NPs are uniformly dispersed on the silica surface with a metallic particle size of 4–6 nm, which exist as metallic Pd and Pt on the surface of monodisperse KCC-1, showing the transfer of electrons from Pd to Pt. The as-synthesized 2.5%Pt-2.5%Pd/KCC-1 exhibited excellent catalytic activity and stability for the continuous dehydrogenation of 2-methoxycyclohexanol to prepare guaiacol. Compared with Pt or Pd single metal supported catalysts, the obtained 2.5%Pt-2.5%Pd/KCC-1 shows 97.2% conversion rate of 2-methoxycyclohexanol and 76.8% selectivity for guaiacol, which attributed to the significant synergistic effect of bimetallic Pt-Pd alloy NPs. Furthermore, turn over frequency value of the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs achieved 4.36 s –1 , showing higher catalytic efficiency than other two monometallic catalysts. Reaction pathways of dehydro-aromatization of 2-methoxycyclohexanol over the obtained catalyst are proposed. Consequently, the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs prove their potential in the dehydrogenation of 2-methoxycyclohexanol, while the kinetics and mechanistic study of the dehydrogenation reaction over the catalyst in a continuous fixed-bed reactor may provide valuable information for the development of green, outstanding and powerful synthetic pathway of guaiacol.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Ping Yu,Lin Wang,Huan Liu,Anfeng Yu,Xinmei Liu,Zhe Yang
Developing reliable and cost-effective optical hydrogen sensors detecting hydrogen leakage at room temperature is of paramount importance. It requires that hydrogen sensors show a rapid and significant color change in low concentration H 2 /air mixtures, which remains challenging. Herein, we demonstrate an eye-readable hydrogen sensor based on Pt decorated hexagonal WO 3 (W 0 /300/Pt). It is evidenced W 0 /300/Pt exhibits excellent gasochromic properties, with reflectivity differences of 78% and 73% and fast coloring times of 3.10 s and 2.64 s in 10% H₂/Ar and 10% H₂/air. Moreover, W 0 /300/Pt shows an obvious color change from light gray to dark blue finally with ΔE value of 71, and exhibits a detect limitation less than 0.1% H 2 in 1 s. The gasochromic mechanism related to crystalline phase structure was unveiled via in situ characterization techniques. This study also presents novel evidence that bolsters the “localized water molecules” model and provides theoretical insights for the advancement of highly sensitive WO 3 gasochromic materials.
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Frontiers in Energy
·
2025
·
IF 6.2
Tang Wenbin,Xia Shuyue,Chou Haiwen,Zhao Jianan,Zhou Yi,Huang Qinghong,Yu Nengfei,Wu Yuping
The oxygen reduction reaction (ORR) plays a crucial role in key processes of fuel cells and zinc-air batteries. To enable commercialization, reducing the platinum (Pt) content and increasing the specific activity per unit mass is essential. A promising approach involves synthesizing of Fe-N-C precursors via the polyaniline (PANI) pathway, which ensures a uniform distribution of Fe-N-C species and facilitates the subsequent adsorption of platinum ions. This leads to the formation of Pt-Fe bimetallic alloys. The synergistic interaction between Pt and Fe-N-C sites promotes the homogeneous dispersion of Pt and the formation of smaller particle sizes, which in turn enhances intrinsic activity and stability of the catalyst. Notably, the Pt/Fe-N-C catalyst, featuring an ultra-low Pt loading of just 1.79 wt%, exhibits a remarkable doubling of mass activity compared to conventional catalysts. Moreover, zinc-air batteries using this catalyst achieve an impressive peak power density of 200 mW/cm 2 .
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APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Ting Yi,Yibo Zhang,Xiangguang Yang
Pt@CeO 2 /MCM-56 (PCM) and CeO 2 -CuO (9:1)/MCM-56 (CCM) were combined to purify the exhaust emissions from diesel vehicles in three configuration statuses, defined as configuration A—where CCM stays above PCM, configuration B—where PCM stays above CCM, and configuration C—where CCM mixes with PCM homogeneously in loose contact. Among these combined catalysts, the configuration A is most favorable for the selective catalytic reduction (SCR) reaction, with >80% NO x conversion obtained at the temperature range of 150–550 °C and gas hourly space velocity (GHSV) of 240,000 ml g −1 h −1 . NH 3 -TPD, H 2- TPR and NH 3 conversion measurements demonstrated that NH 3 can be selectively used to reduce NO x in the configuration A but is over-oxidized if the reaction is operated in configuration B or configuration C status, deteriorating the deNO x activity at temperature above 250 °C. Hence, configuration A not only takes advantage but also overcomes the shortcomings of PCM and CCM, leading to high NO x conversion and N 2 selectivity. A significant decrease in the onset temperature of soot combustion was also observed in this research.
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ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Guiqiang Wang,Shuai Kuang,Juan Zhang,Shuo Hou,Siming Nian
A graphitic carbon nitride (g-C 3 N 4 )/multiwalled carbon nanotubes (MWCNT) composite is prepared by a combination of refluxing process and heating polymerization and investigated as the counter electrode in dye-sensitized solar cells. SEM and TEM studies indicate that MWCNT is very well incorporated and attached to g-C 3 N 4 . Electrochemical impedance spectroscopy demonstrates that the charge-transfer resistance of g-C 3 N 4 /MWCNT composite electrode is 2.1 Ω cm 2 , which is much lower than those of the individual g-C 3 N 4 and MWCNT electrodes. This enhanced electrocatalytic activity is beneficial for improving the photovoltaic performance of dye-sensitized solar cells. Under illumination of 100 mW cm −2 , the dye-sensitized solar cell based on g-C 3 N 4 /MWCNT counter electrode achieves a conversion efficiency of 6.34%, which is comparable to that of the cell based on Pt counter electrode.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 10
·6316-6324
·
IF 12.732
Kun Xiang,Zhongxin Song,Dan Wu,Xiaohui Deng,Xuewan Wang,Wen You,Zhikun Peng,Lei Wang,Jing-Li Luo,Xian-Zhu Fu
Electrocatalytic seawater splitting has been considered as a transformative technology for industrial-scale hydrogen generation. However, the competition between the oxygen evolution reaction (OER) and chlorine evolution reaction (CER) at the anode with sluggish kinetics is the main bottleneck. Herein, an organic-oxidation-assisted strategy has been demonstrated, in which the thermodynamically favorable methanol selective oxidation reaction (MSOR) is used to suppress the undesired OER/CER using carbon paper supported Pt–Co3O4 electrocatalysts (denoted as Pt–Co3O4/CP), leading to hydrogen and value-added formate generation simultaneously with significantly low energy consumption. In the integrated two-electrode electrolyzer using Pt–Co3O4/CP bifunctional electrocatalysts, the required cell voltage at 10 mA cm−2 is only 0.555 V when adding 2.0 M methanol, which is 1022 mV lower than that in alkaline seawater. The integrated cell also produces hydrogen and formate simultaneously with high faradaic efficiency and considerable durability. The findings in this work represent a new direction for energy-saving production of hydrogen from seawater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Shiyue Ren,Yingnan Duan,Zhimin Feng,Haitao Yuan,Lihong Hu,Jiao Wang,Weizun Li,Zhurui Shen
Photocatalytic CO 2 reduction is a promising approach to close the carbon cycle by converting CO 2 into high-value chemicals and fuels, but its practical advancement is hindered by key challenges in photocatalyst design. Though oxygen vacancies (O V ) engineering and noble metal co-catalysts can enhance performance via synergistic strong metal-support interactions (SMSI), their use is limited by harsh synthesis conditions and noble metal cost. Herein, we integrated Pt nanoparticle (Pt NPs )-loaded mixed-phase TiO 2 (anatase/rutile) with abundant O V via a facile two-step method. The as-prepared Pt/A2-TiO 2-x exhibited CH 4 and CO production rates of 72.31 and 55.45 μmol·g⁻¹·h⁻¹ in pure H 2 O, representing 5.6- and 9-fold enhancements over pristine TiO 2 . Characterizations, theoretical calculations, and in-situ Fourier transform infrared spectroscopy confirmed that O V facilitated robust Pt-TiO 2 SMSI, which promoted bulk photogenerated electron migration to Pt surfaces and accelerated CO 2 adsorption/activation, thereby optimizing the CO 2 -to-CH 4 reaction pathway. This work deepens understanding of metal-vacancy synergy and provides a rational strategy for designing cost-effective, high-performance photocatalysts for CO 2 reduction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Bowen Yang,Yangyang Long,Feng Chen,Jiabao Wang,Zhipeng Wang,Ziqiang Zhang,Yanfei Wang,Weihua Zou,Yeguang Zhang,Peng Wang,Zili Zhan,Feihu Li
Hydrogen sensor based on proton exchange membrane fuel cells (PEMFCs) was one of the most extensively studied types. However, traditional Pt/C based electrodes suffered from several drawbacks, including high cost, low catalytic efficiency for oxygen reduction reaction (ORR) and slow reaction kinetics. Herein, we developed a quasi PEMFCs hydrogen sensor utilizing MnO 2 as cathode catalyst, where the electrochemical signal was generated via the direct MnO 2 redox reaction with hydrogen, replacing the ORR process. Membrane electrode assemblies (MEAs) were successfully fabricated incorporating α-MnO 2 , β-MnO 2 , and δ-MnO 2 polymorphs. The β-MnO 2 -based sensor demonstrated best sensing performance with a maximum sensitivity of 96 nA/ppm, a 34-fold enhancement over conventional dual-platinum electrochemical sensors, under the optimized volume ratio of catalyst ink (ethylene glycol: Nafion solution: water = 1:4:4). Moreover, the β-MnO 2 -based sensor exhibited significantly superior response and recovery speed. This strategy provided an effective approach for the commercialization of next generation PEMFCs-type hydrogen sensors.
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FUEL
·
2025
·
IF 7.5
Fan Shao,Fengzhi Guo,Tianyu Bai,Zhen Xu,Han Yang,Wenbo Kang,Yasong Zhou,Wenbin Huang,Gang Wang,Qiang Wei
The inherent diffusion constraints imposed by narrow micropores and elongated channels in Y zeolites severely limit jet fuel selectivity during Fischer-Tropsch wax hydrocracking. Advanced supports were synthesized via seed-directed crystallization (nano-Y-0P zeolite) and PDDA (polydiallydimethyl ammonium chloride)-mediated assembly (hierarchical nano-Y-xP zeolites, x = 0.1, 0.3, 0.6, 0.9). This dual-strategy synergistically addresses diffusion constraints in conventional Y-zeolite by optimizing nano structure of active sites and improving interfacial mass transfer (i.e., nano-crystal size and hierarchical porosity). Intelligent Gravimetric Analysis (IGA) directly validates hierarchical porosity and nanocrystalline advantages. Y-0.6P zeolite with optimal mesoporosity (0.75 cm 3 /g vs. 0.25 cm 3 /g in conventional Y-zeolite) and minimal crystallite size (131 nm vs. 1258 nm in conventional Y-zeolite) achieves intrinsic diffusion enhancement—the 5.36-fold higher diffusion rate than conventional S-Y zeolite. Zeolite crystallite size and hierarchical porosity critically govern metal–acid functionality balance by modulating acid site density (589.7 μmol/g vs. 812.4 μmol/g in conventional Y zeolite) and optimizing metal dispersion (40.5 %, vs. 18.26 % in conventional Y-zeolite). Pt/(Y-0.6P+ASA) catalyst achieves peak performance with 35.04 % C 9 –C 17 yield and 47.35 % selectivity in n-docosane hydrocracking. Notably, Fischer-Tropsch wax hydrocracking yields 26.83 % jet fuel (49.88 % selectivity) with ideal bell-shaped distribution. This work demonstrates Y-0.6P-supported catalyst has industrial potential for aviation fuel production from Fischer-Tropsch wax upgrading.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 35
·13967-13978
·
IF 3.069
Qiang Ning,Huaike Zhang,Yurong He,Zhiqiang Chen,Suyao Liu,Jie Ren
Small Pt particles (about 1.2 nm) were highly dispersed on ZSM-22 zeolites via a strong electrostatic adsorption (SEA) method and exhibited a promotion effect on the catalytic performance in n-dodecane isomerization in comparison with the conventional catalyst. Several promoters (Ce, La, and Re) were introduced to further improve the aggregation resistance of the small Pt particles. A series of characterization including H2-TPR, XPS and STEM as well as DFT calculations provided solid evidence that the strong interaction between Pt and promoter species not only effectively hinders the Pt aggregation but also alters the electronic state of the Pt sites. Moreover, Ce and La promoters also lead to a slightly improved amount of B acid sites determined by Py-FTIR. Thus, improved activity and selectivity were achieved on a Ce-modified catalyst due to the better balanced bifunctionality between the slightly increased acidity of zeolites and electron-deficiency of Pt. The electron-rich Pt sites are responsible for the significant increase of CH4 selectivity and the decrease of total isomer selectivity in n-dodecane isomerization. In addition, a high-temperature reduction test revealed the higher isomerization activity and selectivity (about 10% higher than the unmodified catalyst) of the Ce-modified catalyst owing to the strong bond of Pt–O–Ce, further confirming the positive effect of the Ce promoter on the sintering resistance of small Pt particles.
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RSC Advances
·
2016
·Vol. 6
·期 74
·70303-70310
·
IF 3.289
Hongxing Zhang,Yiwei Zhang,Yuming Zhou,Chao Zhang,Xiaoli Sheng,Shuo Zhao,Jiasheng Fang,Mingyu Zhang
This article reports a facile and controllable one-step method to construct Pt@hollow mesoporous SiO2 (Pt@HMSiO2) nanoparticles (NPs). To enhance the catalytic activity, cerium species were impregnated into Pt@HMSiO2 NPs, fabricating highly reactive Pt–CeO2@HMSiO2 NPs. To verify the successful synthesis of the Pt@HMSiO2 and Pt–CeO2@HMSiO2 NPs, and study the influence of CeO2 species on the catalytic performance, the as-prepared NPs were characterized by several techniques, including SEM, TEM, EDX, FTIR, XRD, BET and UV-vis analyses. In this work, the reduction of 4-NP was employed as a model reaction to test the catalytic performance. Compared to Pt@HMSiO2, the Pt–CeO2@HMSiO2 NPs show higher catalytic activity, because of the co-catalysis of CeO2 NPs. However, the excess amount of CeO2 NPs would lead to a lower catalytic activity, due to the blocking of the catalyst pore. In addition, the Pt–CeO2@HMSiO2 NPs show a high thermal stability due to the protection of the SiO2 shell. Meanwhile, we have also used the reaction of propane dehydrogenation to further verify the excellent catalytic stability of Pt–CeO2@HMSiO2 NPs. This strategy is novel, albeit efficient, and can be extended to the preparation of other nanocatalysts.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Aicaijun Zhang,Pengyu Dong,Yan Wang,Kangjie Gao,Jinkang Pan,Bairen Yang,Xinguo Xi,Jinlong Zhang
It is still challenging to fabricate photocatalysts via loaded metal cocatalysts with good dispersion onto the conjugated polymers (CPs). Herein, a donor-acceptor (D–A) structural CP of PyDTDO-3 was employed to host platinum (Pt) nanoparticles (NPs) using N , N ′-dimethylformamide (DMF) as a protectant, stabilizer, and reducing agent, which not only promotes Pt NPs to have excellent dispersion property on the surface of PyDTDO-3 but also endows Pt NPs to maintain metallic Pt 0 species. As a result, the PyDTDO-3 loaded with Pt NPs exhibits remarkable hydrogen (H 2 ) evolution activity with a rate of 39.9 mmol g −1 h −1 under visible light irradiation, and the fair stability of optimal 7% Pt/PyDTDO-3 is expressed in the rate of H 2 generation upon 30 h cycling. Based on density functional theory (DFT) calculations, it has been demonstrated that Pt NPs are selectively loaded onto the acceptor (A) unit of PyDTDO-3 that has the lowest adsorption energies ( E ads ) and the closest bond lengths between the Pt NPs and PyDTDO-3. Moreover, there are much more electrons filling at the Fermi level ( E f ), indicating the optimal 7% Pt/PyDTDO-3 with high electroconductivity timely captured and removed the photoinduced electrons and thus realized the space separation efficiency of electron-hole pairs. Overall, our findings offer a rational way to load metal cocatalysts onto CPs with good dispersion for efficient photocatalytic H 2 evolution.
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