SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Hao Wu,Jun Yu,Zhongzhou Li,Guanyu Yao,Rui Cao,Xiaogan Li,Huichao Zhu,Aixiang He,Zhenan Tang
High-performance, low-power microhotplate (MHP) gas sensors loaded with 3D hierarchical structured PdO/PdO 2 -SnO 2 :Sb materials on a pair of Al gas sensing electrodes were fabricated through advanced high-accuracy electrohydrodynamic printing method. The PdO/PdO 2 -SnO 2 :Sb materials with various PdO/PdO 2 concentrations were initially synthesized via a mild and simple hydrothermal reaction. Their micromorphology and chemical composition were characterized by SEM, XRD, TEM, and XPS, which proved the successful synthesis. The gas sensing performance of the sensors to benzene, ethanol, acetone, formaldehyde, and ethanol-acetone mixed gas (volume ratio 1:1) was tested. The sensing property of the materials is regulated with different content of PdO/PdO 2 . The identification of the VOCs is realized by two-step principal component analysis (PCA). Simulation calculations on the I–V characteristic of the MHP gas sensors reveal that carriers have to get through Al 2 O 3 barriers by Poole-Frenkel emission, which significantly affects the carrier conduction as well as the gas sensing properties. The gas sensing mechanism is analyzed from the aspects of gas sensing material and electrodes.
研究领域:
材料科学
·
传感器技术
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiacheng Xu,Bo Zhang,Yongkang Lu,Leigang Wang,Wanyi Tao,Xiao Teng,Wensheng Ning,Zekai Zhang
Preparation of PdO/SiO 2 @graphene oxide (GO) hybrid aerogels were carried out sol-gel method combined with atmospheric drying technology to study their adsorption performance for thiophenics and compared with PdO/SiO 2 . Scanning electron microscope (SEM), N 2 adsorption-desorption isotherms, X-ray diffraction (XRD) analysis, X-ray photoelectron spectroscopy (XPS), and fourier transformation infrared spectroscopy (FT-IR) for samples were performed. The adsorption performance of PdO/SiO 2 @GO for thiophene were better than that of PdO/SiO 2 , attributed to that incorporation of GO increased the specific surface area and the Pd incorporation rate, where Pd 2+ ions acted as the π-complexation and sulfur-metal (S M) bond adsorption active centers, as well as GO adsorbed thiophene by the π-π stacking effect. The adsorption capacities of PdO/SiO 2 @GO-1.0 for thiophene (TH), benzothiophene (BT) and dibenzothiophene (DBT) were 8.89, 9.3 and 12.6 mg-S/g ads , respectively. The addition of GO in aerogels could improve the inhibition effect of toluene, cyclohexene and pyridine while decreased the inhibition effect of MTBE and H 2 O for the adsorption of thiophene, due to the π-π stacking effect and the hydrophobicity of GO, respectively. The adsorption process was spontaneous and exothermic, be well fitted by the apparent second-order kinetic model and dominated by chemical interaction. Pd/SiO 2 @GO-1.0 had a good solvent elution regeneration performance.
研究领域:
材料科学
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化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Lei Zhou,Sai Ma,Meizhen Gao,Boyao Xie,Qi Shi
1,3-propanediol (1,3-PDO) is a high-value chemical that can be produced via glycerol hydrogenolysis or biological fermentation. The main products of glycerol hydrogenolysis include 1,3-PDO and 1,2-propanediol (1,2-PDO). The properties of propanediol isomers are extremely similar, which are difficult to effectively separate them. Based on the differences in the shape of ellipsoidal 1,3-PDO and spherical 1,2-PDO, ZIF-300 with a 6-member ring (6-MR) trap between cha and d6r cages that can match spherical 1,2-PDO have been selected for the separation of propanediol isomers. ZIF-300 series materials (named ZIF-300-S1, ZIF-300-S2 and ZIF-300-S3) with different 6-MR trap orientations have been constructed by variable the ratio between the small-sized 2-methylimidazole (mIm) and large-sized 5-bromobenzimidazole (bbIm) links. Theoretical and experimental results show that ZIF-300-S3 (Zn(mIm) 1.04 (bbIm) 0.96 ) preferentially adsorbed 1,2-PDO over 1,3-PDO because the 6-MR trap with uniform large bbIm/small mIm links distribution faces essentially the small d6r cage, which can better match spherical 1,2-PDO. In contrast, ZIF-300-S1 (Zn(mIm) 0.82 (bbIm) 1.18 ) show low uptake of 1,2-PDO and 1,3-PDO because the 6-MR trap with main large bbIm links distribution faces essentially the larger cha cage, which show weak confinement of 1,2-PDO and 1,3-PDO. The dynamic column adsorption (1,2-PDO/1,3-PDO: 50/50 g L −1 ) results exhibited that the adsorption capacity of ZIF-300-S3 for 1,2-PDO can be as high as 64.7 mg g −1 and selectivity for 1,2-PDO/1,3-PDO was 2.0. This work provides valuable insights into the construction of ZIFs materials with tunable 6-MR trap for effective separation of isomers.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Xiangyu Ma,Hui Xu,Zhang Liu,Yanfei Liu,Chen Wang,Meiqing Shen,Chun Du,Bin Shan
Catalytic oxidation is a valuable residual methane removal method, and Pd-based catalysts are the most robust and widely applied system. Yet, they suffer from poor stability in practical applications due to sintering and water poisoning. In this work, we prepared a high-performance PdNi/Al2O3 catalyst with PdO-NiO and PdO-NiAl2O4 dual interfaces. PdNi/Al2O3 showed excellent hydrothermal stability after aging at 750 °C, 10% H2O for 72 h, with the T50 remaining below 315 °C. In addition, compared to bare Pd/Al2O3, PdNi/Al2O3 exhibited a better low-temperature activity with a T50 of 287 °C, rivaling state-of-the-art Pd-based catalysts. Combining structural characterizations and DFT calculations, it was shown that dual interfaces promoted the activation of methane C–H bonds and suppressed the adsorption of surface water/hydroxyl groups and agglomeration of PdO particles. This study has provided new perceptions for exploring the influence of interfacial interactions and offered a route to synthesize high-stability palladium catalysts.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
ACS Applied Energy Materials
·
2024
·
IF 5.4
Heng Chen,Li Li,Shichao Zhang,Chaofeng Zhang
Recently, as an important product of the CO2 hydrogenation reaction and a crucial hydrogen storage material, the transformation of formic acid (FA)/formate to H2 or active hydrogen species has attracted much attention. However, obtaining a robust and efficient solid catalyst constitutes a major challenge. In this work, nitrobenzene was used as the active hydrogen species capture agent, and various Pd-based catalysts were prepared and used to refine the influence factors of FA decomposition over TiO2-supported palladium catalysts. The catalysts’ deactivation and regeneration process, control reactions, and catalyst characterizations indicate that the electrical state of the Pd species and interface microsurroundings played decisive roles in the activity and reusability of PdO/TiO2. Based on the results obtained, a tentative mechanism with the active sites (Pdδ+–O–Ti) located at the PdO/TiO2 interface was proposed, which would be useful for the chemistry of the Pd catalyst and formate decomposition.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Fanggang Zhang,Sheng Su,Juan Wang
Aiming to achieve efficient utilization of high-energy–density fuels in the promising portable power systems, self-sustained combustion of n-decane over Co 3 O 4 -based catalysts in a narrow quartz reactor was investigated. Chemiluminescence, gas chromatography and various physicochemical characterization methods were used in this study. The evidences suggest that Co 3 O 4 -based catalysts can significantly reduce the ignition temperature and broaden the flammability limits of n-decane. The heat release stored in the catalyst bed can help improve the flame stability, delay the flame extinction, and achieve auto-ignition without forced heating. Besides, great promotion of the catalytic performance of Co 3 O 4 spinel is achieved by doping with 6 wt% PdO. PdO/Co 3 O 4 catalysts exhibit higher activity and enhanced ability in effectual resistance toward deactivate than pure Co 3 O 4 . Furthermore, the coupling of heterogeneous and homogeneous reactions of n-decane has been analyzed. It can be revealed that both the adsorbed and gaseous OH* radicals play greatly different roles when using different catalysts. These findings promote the use of heavy hydrocarbon fuels for energy supply and contribute to designing efficient Co 3 O 4 -based catalysts rationally.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2021
·
IF 5.565
Chang Cui,Yan Zhang,Wenpo Shan,Yunbo Yu,Hong He
Alumina supported Pd catalyst (Pd/Al 2 O 3 ) is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900°C and isothermal experiments at 650°C were conducted to investigate the influence of NO x on transient deactivation of Pd/θ-Al 2 O 3 catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient deactivation in the cooling ramp from 800 to 500°C, which was resulted from the in situ formation of NO 2 during the process of methane oxidation. Over the Pd/θ-Al 2 O 3 , thermogravimetric analysis and O 2 temperature programmed oxidation measurements confirmed that transient deactivation was due to the decomposition of PdO particles and the hysteresis of Pd reoxidation, while the metal Pd entities were less active for methane oxidation than the PdO ones. CO pulse chemisorption and scanning transmission electron microscopy characterizations rule out the NO 2 effect on Pd size change. Powder X-ray diffraction and X-ray photoelectron spectroscopy characterizations were used to obtain palladium status of Pd/θ-Al 2 O 3 before and after reactions, indicating that in lean conditions at 650°C, the presence of NO 2 increases the content of active PdO on the catalyst surface, thus benefits methane oxidation. Homogeneous reaction between CH 4 , O 2 , and NO x may be partially responsible for the alleviation above 650°C. The interesting research of alleviation in transient deactivation by NO x , the components co-existing in exhausts, are of great significance for the application.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 3
·325
·
IF 4.501
Qinglei Meng,Xiaolong Yang,Xian Wang,Meiling Xiao,Kui Li,Zhao Jin,Junjie Ge,Changpeng Liu,Wei Xing
Formic acid decomposition (FAD) is one of the most promising routes for rapid hydrogen (H2) production. Extensive efforts have been taken to develop efficient catalysts, which calls for the simultaneous regulation of the electronic structure and particle size of the catalyst. The former factor determines the intrinsic performance, while the latter corresponds to the active site utilization. Here, an effective preparation strategy, pre-nucleation coupled with in situ reduction, is developed to realize and well-tune both surface electronic states and particle size of the pallidum (Pd) catalyst. Benefiting from the structural merits, the as-prepared catalyst exhibits high mass-specific activity of 8.94 molH2/(gPd·h) with few carbon monoxide (CO) molecules, and the activation energy could reach a value as small as 33.1 kJ/mol. The work not only affords a highly competitive FAD catalyst but also paves a new avenue to the synthesis of ultra-fine metal nanoparticles with tailorable electronic structures.Keywords:hydrogen evolution;formic acid;heterogeneous catalysis;high selectivity;Pd-PdO interface
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Decun Luo,Ziyu Tang,Xiyang Yu,Tao Zhang,Chun-Ran Chang,Zhun Hu
The effect of ZrO 2 crystalline phases on Pd/ZrO 2 for catalytic combustion of toluene was investigated. It was found that Pd/t-ZrO 2 showed superior activity when the toluene concentration was lower than 2000 ppm, while Pd/m-ZrO 2 performed better with toluene concentration higher than 3000 ppm. Kinetic studies showed that the reaction order of toluene on Pd/t-ZrO 2 and Pd/m-ZrO 2 is 0 and 2, respectively. The catalytic activity was controlled by combined effect of PdO activity and quantity, which was correlated with the interaction between palladium and zirconia. The t-ZrO 2 increased PdO species activity, while m-ZrO 2 could enhance the amount of PdO. DFT results showed that the p-band center of the O of PdO on t-ZrO 2 was higher, suggesting that PdO was more active. In situ -DRIFTS revealed that the reaction pathway of catalytic oxidation of toluene on Pd/ZrO 2 was as follows: toluene was oxidized stepwise to benzyl alcohol, benzaldehyde, benzoic acid , CO 2 and H 2 O.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 56
·29563-29570
·
IF 3.708
Jingjing Lin,Tao Mei,Meijiao Lv,Chang'an Zhang,Zhenfeng Zhao,Xianbao Wang
A simple two-step method for the preparation of Pd nanoparticles supported on reduced graphene oxide (Pd/RGO) is reported. Well-dispersed and size-controlled Pd/RGO was synthesized through reduction of PdO nanoparticles on graphene oxide (PdO/GO) with hydrazine hydrate and ammonia at 80 °C for 4 hours. The PdO/GO was successfully prepared by mixing GO and Pd(NO3)2 aqueous solution together without adding any additional chemicals. The sizes and morphologies of PdO nanoparticles can be controlled by changing the concentrations of Pd(NO3)2, reaction temperatures and times. The results suggest that a small scale increase of the loadings of Pd supported on RGO can significantly improve the catalytic activity of Pd/RGO, and the stability is much better than that of commercial Pd/C catalysts for methanol electrooxidation and the Suzuki reaction.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 36
·期 13
·e17378
·
IF 19
Zhenxu Li,Tongtong Qi,Xinhua Zhao,Yi Zhang,Zhu Zhang,Tingting Wang,Xuze Xiao,Dachi Yang
Reliable methane (CH 4 ) sensing is highly desired in the underground pipe networks, and even low-concentration CH 4 leakage may cause disasters. However, it often suffers from instability and sluggish response caused by harsh working conditions (e.g., high humidity). Here, cerium oxide hollow nanospheres decorated with palladium and palladium oxide nanodots (Pd-PdO NDs / CeO 2 HNSs) are reported for stable and fast CH 4 sensing, which have been prepared via combined bubble confinement and in situ photochemical deposition. As-prepared Pd-PdO NDs / CeO 2 HNSs are hollow nanospheres of ≈0.96 µm in diameter. Beneficially, the sensing materials exhibit 3 s fast response and 0.1 ppm limit of detection. Further, Pd-PdO NDs / CeO 2 HNSs show excellent sensing stability of 510 days stability, 74% relative humidity tolerance, and 100 cycling stability. Theoretically, such outstanding CH 4 sensing performance is attributed to interface-coupled modulation between Pd-PdO NDs and CeO 2 HNSs, in which Pd-PdO NDs serve as catalytic centers, while CeO 2 HNSs act as both oxygen vacancy modulator and structural optimizer. Compared with a commercial sensor, Pd-PdO NDs / CeO 2 HNSs present superior response / recovery time, and a sensor prototype has been built to simulate the detection of CH 4 leakage with reliable responses.
✓ 已验证
DOI
高影响因子
Nanomaterials
·
2024
·Vol. 14
·期 14
·1188
·
IF 4.4
Hongyang Wu,Chen Chen
The efficient detection of n-butanol, which is in demand for highly sensitive materials, is essential for multiple applications. A nonaqueous method was applied to prepare NiFe2O4nanoparticles (NPs) using benzyl alcohol as a solvent, which shows a size of 7.9 ± 1.6 nm and a large surface area of 82.23 m2/g. To further improve the sensing performance for n-butanol, Pd/PdO functionalization was sensitized with NiFe2O4NPs. Gas sensing results demonstrate that the Pd/PdO-NiFe2O4exhibits an enhanced response of 36.9 to 300 ppm n-butanol and a fast response and recovery time (18.2/17.6 s) at 260 °C. Furthermore, the Pd/PdO-NiFe2O4-based sensor possesses a good linear relationship between responses and the n-butanol concentration from 1 to 1000 ppm, and great selectivity against other volatile organic compounds (VOCs). The excellent sensing enhancement is attributed to the catalytic effects of Pd/PdO, the increase of oxygen vacancies, and the formation of heterojunction between PdO and NiFe2O4. Thus, this study offers an effective route for the synthesis of Pd/PdO-functionalized NiFe2O4NPs to achieve n-butanol detection with excellent sensing performance.
研究领域:
材料科学
·
化学传感器
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）