Journal of Energy Chemistry
·
2023
·
IF 13.1
Yuling Chen,Yali Wen,Qun Zhou,Lina Shen,Fanghui Du,Pai Peng,Yu Chen,Junwei Zheng
Herein, Pd nanoparticles loaded Co 3 O 4 catalysts (Pd@Co 3 O 4 ) are constructed from zeolitic imidazolate framework-67 (ZIF-67) for the ethanol oxidation reaction (EOR). It is demonstrated for the first time that the electrochemical conversion of Co 3 O 4 support would result in the charge distribution alignment at the Pd/Co 3 O 4 interface and induce the formation of highly reactive Pd-O species (PdO*), which can further catalyze the consequent reactions of the intermediates of the ethanol oxidation. The catalyst, Pd@Co 3 O 4 -450, obtained under the optimized conditions exhibits excellent EOR performance with a high mass activity of 590 mA mg −1 , prominent operational stability, and extraordinary capability for the electro-oxidation of acetaldehyde intermediates. Importantly, the detailed mechanism investigation reveals that Pd@Co 3 O 4 -450 could be benefit to the C–C bond cleavage to promote the desirable C1 pathway for the ethanol oxidation reaction. The present strategy based on the metal-support interaction of the catalyst might provide valuable inspiration for the design of high-performing catalysts for the ethanol oxidation reaction.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Catalysts
·
2019
·Vol. 9
·期 5
·410
·
IF 3.444
Lei Ma,Shiyan Yuan,Taotao Jiang,Xiangming Zhu,Chunshan Lu,Xiaonian Li
Sulfur species (e.g., H2S or SO2) are the natural enemies of most metal catalysts, especially palladium catalysts. The previously reported methods of improving sulfur-tolerance were to effectively defer the deactivation of palladium catalysts, but could not prevent PdO and carrier interaction between sulfur species. In this report, novel sulfur-tolerant SiO2supported Pd4S catalysts (5 wt. % Pd loading) were prepared by H2S–H2aqueous bubble method and applied to catalytic complete oxidation of methane. The catalysts were characterization by X-ray diffraction, Transmission electron microscopy, X-ray photoelectron Spectroscopy, temperature-programmed oxidation, and temperature-programmed desorption techniques under identical conditions. The structural characterization revealed that Pd4S and metallic Pd0were found on the surface of freshly prepared catalysts. However, Pd4S remained stable while most of metallic Pd0was converted to PdO during the oxidation reaction. When coexisting with PdO, Pd4S not only protected PdO from sulfur poisoning, but also determined the catalytic activity. Moreover, the content of Pd4S could be adjusted by changing H2S concentration of H2S–H2mixture. When H2S concentration was 7 %, the Pd4S/SiO2catalyst was effective in converting 96% of methane at the 400 °C and also exhibited long-term stability in the presence of 200 ppm H2S. A Pd4S/SiO2catalyst that possesses excellent sulfur-tolerance, oxidation stability, and catalytic activity has been developed for catalytic complete oxidation of methane.
研究领域:
催化化学
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环境催化
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材料化学
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能源化学
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表面科学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Yun Zhang,Guangfei Qu,Yaoze Wang,Zhishuncheng Li,Junhong Zhou,Ping Ning,Nanqi Ren
This study investigates the modification of electrode materials to improve their activity and selectivity in the CER by magnetizing ferromagnetic electrode materials, thereby inducing spin polarization of electrons on the material surface. The experimental data demonstrate that in a 2 M NaCl solution (pH = 6) under a constant current density of 10 mA cm −2 , the CNP/CC electrode exhibited overpotentials that were lower by 33 mV and 73 mV prior to and following magnetization, respectively, in comparison to the standard DSA electrode. In the 300-s electrolysis test, the CNP/CC electrode exhibited Faraday efficiencies of 85.13% prior to magnetization and 94.32% following magnetization. These findings demonstrate that the CNP/CC electrode outperforms the conventional dimensionally stable anodes (DSA) electrode in terms of overpotential, highlighting the significant role of magnetization treatment in enhancing electrocatalytic performance. The CNP/CC electrode exhibited excellent stability, with only a slight potential change (from 1.14 V to 1.19 V vs. RHE) after 24 h of continuous stability testing. Notably, the CNP/CC electrode was synthesized using only 0.0304%wt of the precious metal palladium, substantially reducing the manufacturing cost of the chlorine evolution electrode and offering an efficient and cost-effective electrode material for the chlor-alkali industry.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
VACUUM
·
2025
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IF 3.9
Xiaohua Wang,Yanwei Li,Xinhui Jin,Guang Sun,Jianliang Cao,Yan Wang
The pressing need for health and environmental protection has sparked significant interest among researchers in exploring gas sensors made from metal oxide semiconductors (MOSs). Herein, a co-modification approach involving palladium (Pd) and palladium oxide (PdO) is introduced to enhance the sensing properties of indium oxide (In 2 O 3 ) to hydrogen sulfide (H 2 S). Pd and PdO co-modified In 2 O 3 hierarchical porous nanocubes (Pd/PdO-In 2 O 3 HPNCs) were synthesized using a facile hydrothermal method. With the theoretical doping amount of 2 mol%, the synergistic effect of metal Pd and PdO-In 2 O 3 heterojunction made Pd/PdO-In 2 O 3 show excellent sensing performance to H 2 S compared to In 2 O 3 . Specifically, the material features a lower operating temperature (280 vs 300 °C), higher sensitivity (95.06 vs 28.59 to 20 ppm H 2 S; 2.28 vs 1.17–100 ppb H 2 S), and better selectivity (7.41 vs 2.32 times to triethylamine), while also demonstrating satisfactory reproducibility and stability. The synergistic sensitization mechanism of noble metal catalysis and heterojunction in Pd/PdO–In 2 O 3 HPNCs, along with their underlying mechanism, was discussed. Integrating noble metal modification with heterojunctions adds complexity to the structure and composition of the material. The synergistic effects of these two sensitization strategies on the H 2 S sensitization mechanism need further in-depth investigation.
研究领域:
材料科学
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化学传感器
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纳米技术
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环境监测
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半导体物理
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产品关联
DOI
高影响因子
POLYMER
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2026
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IF 5.1
Chang Liu,Yuming Cui,Yunbo Mo,Qian Xu,Kai Wang,Jianwu Lan,Shaojian Lin
Commercial poly(butylene adipate-co-terephthalate) (PBAT), a biodegradable aromatic–aliphatic copolyester, is considered a promising alternative to conventional plastics in various fields. However, its relatively low mechanical strength and low glass transition temperature (T g ) often restricts broader applications. In this study, bio-based 1,3-propanediol (PDO) was employed to completely replace 1,4-butanediol in PBAT, and a series of poly(trimethylene terephthalate- co -trimethylene adipate) (PPAT) copolyesters were synthesized via melt polycondensation. Structural characterization confirmed the targeted copolyester compositions and random chain segments (R ≈ 1), with intrinsic viscosities of 0.89-1.01 dL/g. Crystallographic analysis revealed that the crystallinity of PPATs varied with the adipic acid/dimethyl terephthalate molar ratio while preserving a monoclinic crystal structure. Notably, PPAT55 exhibited a significantly higher T g (−7.8 °C) than PBAT (−26.1 °C), and all copolyesters showed good thermal stability for melt processing. Importantly, PPAT55 fibers achieved a tensile strength of 0.71 cN/dtex after threefold drawing, representing a 51.06% enhancement over PBAT fibers. Furthermore, the increased aliphatic segment content promoted by hydrolytic susceptibility, as demonstrated by enzymatic degradation tests, with PPAT55 showing a 9.93% mass loss after 42 days, demonstrating satisfactory biodegradability comparable to PBAT. The degradation mechanism was further elucidated at the molecular level through theoretical calculations. This work provides a feasible strategy for developing high-performance sustainable polyester materials with good spinnability.
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
Jiayu Song,Shengping Wang,Yan Xu,Qingling Liu,Yujun Zhao
Poor catalytic activity and stability are primary defects of traditional Pd/Al 2 O 3 catalysts for the low-temperature methane combustion. Herein, we developed a facile way to synthesize a MgAl-LDHs derived MgAl 2 O 4 spinel with good crystalline lattice and high surface area, which was used as support of Pd-based catalysts. Catalysts with Mg/Al ratio of 1/3 presented the highest methane combustion activity. It was found the well-crystallized MgAl 2 O 4 spinel promoted the dispersion and crystallization of PdO due to the strong interaction between PdO and support, and the electrophilicity and basicity originated from Mg doping suppressed the sintering of PdO particles, leading to the excellent performance of Pd/MgAl3. Moreover, these factors also inhibited the formation of surface OH- species, therefore, improved the water resistance. Such a synthesis strategy of the Pd/Mg x Al y derived from LDHs and the roles of MgAl 2 O 4 spinel could pose some meaningful directions for developing high-efficient Pd-based catalysts for the low-temperature methane combustion.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 17
·7035-7041
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IF 3.288
Mufei Liu,Hao Yang,Zewen Xu,Wenlu Ma,Fang Cui,George Lu,Linxu Xu,Tieyu Cui
Based on green chemistry, 3D hierarchical ZnO microflowers (MFs) constructed from layered 2D nanosheets have been designed as carriers to uniformly load PdO/Pd nanoparticles by the calcination of the precursor (ZnO/Pd(II) microflowers) in air. The ZnO/Pd(II) microflowers are prepared by dipping the 3D ZnO MFs in an ethanolic solution of PdCl2 without involving additional agents. The as-prepared 3D hierarchical ZnO microflowers are a stable support to enhance the dispersibility of PdO/Pd nanoparticles to achieve better catalytic performance for the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP). In addition, the synergistic effect between the PdO and Pd nanoparticles is another major driver that promotes the catalytic process. Over 98% of 4-NP is reduced within 7 min. Furthermore, structural analysis of the ZnO/PdO/Pd microflowers can provide useful information for understanding structure-performance relationships.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Zhang Wenqing,Xi Dawei,Chen Yihong,Chen Aobo,Jiang Yawen,Liu Hengjie,Zhou Zeyu,Zhang Hui,Liu Zhi,Long Ran,Xiong Yujie
Oxidative carbonylation of methane is an appealing approach to the synthesis of acetic acid but is limited by the demand for additional reagents. Here, we report a direct synthesis of CH 3 COOH solely from CH 4 via photochemical conversion without additional reagents. This is made possible through the construction of the PdO/Pd–WO 3 heterointerface nanocomposite containing active sites for CH 4 activation and C–C coupling. In situ characterizations reveal that CH 4 is dissociated into methyl groups on Pd sites while oxygen from PdO is the responsible for carbonyl formation. The cascade reaction between the methyl and carbonyl groups generates an acetyl precursor which is subsequently converted to CH 3 COOH. Remarkably, a production rate of 1.5 mmol g Pd –1 h –1 and selectivity of 91.6% toward CH 3 COOH is achieved in a photochemical flow reactor. This work provides insights into intermediate control via material design, and opens an avenue to conversion of CH 4 to oxygenates.
研究领域:
化学工程
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光化学
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材料科学
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催化
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产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Lingcong Li,Xiaojun Liu,Hong He,Ningqiang Zhang,Ziwen Liu,Guizhen Zhang
The MgO-doped hexagonal boron nitride (MgO-h-BN) nanomaterials were designed as a support for Palladium (Pd) catalysts for CO oxidation reaction. The catalytic properties of Pd/MgO(5)-h-BN catalyst was investigated and compared with Pd/h-BN catalyst. Transmission electron microscopy (TEM) results suggested that the PdO nanoparticles with small grain sizes (ca. 8 nm) were effectively dispersed on the surface of MgO, and the MgO were deposited on the h-BN nanosheets in the Pd/MgO(5)-h-BN catalyst. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses revealed that a small amount of Mg 2+ embedded into the B vacancies of h-BN nanosheets in the Pd/MgO(5)-h-BN catalyst. More significantly, a large amount of adsorbed oxygen appeared near the B vacancies of Pd/MgO(5)-h-BN catalyst. The experiments outcomes of diffuse reflectance fourier transform spectra analysis of CO (CO-DRIFT) indicated that the carbonate/formate species were easily decomposed to CO 2 on the Pd/MgO(5)-h-BN catalyst than Pd/h-BN catalyst, which might be a reason why the Pd/MgO(5)-h-BN catalyst had high CO oxidation activity. According to above analyses, we provide a new insight for the MgO-h-BN nanomaterials for Pd catalysts for application in CO oxidation reaction.
研究领域:
催化
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材料科学
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化学
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纳米技术
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Shuangde Li,Tao Wang,Mu Zhou,Shaohua Chai,Linfeng Nie,Zhenjiang Wu,Ning Han,Yunfa Chen
A dual-functional adsorption–catalytic system for elimination of trace toluene is developed and realized over molecular sieve-hosted varied ratio of platinum and palladium catalysts. PtPd/molecular sieve exhibites PdO and PtO 2 around 2–3 nm particles with uniform loading verified by XRD, TEM, Raman and XPS. The adsorption–desorption–catalysis for trace toluene purification is evaluated on the quartz micro-reactor and the self-made electrically heated equipment. 3Pt1Pd/molecular sieve shows toluene adsorption capacity of 18.22 mg/g and desorption efficiency about 77%, together with the maximum desorption temperature at 100 °C. 3Pt1Pd/molecular sieve owns toluene conversion with 38.3% and 100% at 100 and 200 °C, accompanied with the higher CO 2 selectivity of 0.0% and 150.0%, separately, due to the higher Pd 2+ content. The catalyst displays water vapor endurance, reproducibility, and 83.0% carbon balance during the whole adsorption–desorption–catalysis within 150 min, which highlights the sustainable applicability in lean VOCs abatement. Furthermore, the possible catalytic reaction pathway of toluene oxidation is proposed based on the in-situ DRIFTS experiments.
研究领域:
环境科学
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催化
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材料科学
·
化学工程
✓ 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）