INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Chao Hu,Yunong Zhou,Meifang Xiao,Gang Yu
Control of the structure and shape of platinum nanocrystals has recently attracted much attention, mostly due to their specific properties and related catalytic functionalities. However, the realization of platinum nanocrystals with controlled sizes and dominant facet types remains a significant challenge. In this study, platinum nanoparticles with controllable sizes and dominant facets are produced via a simple, organic agent-free, rapid, clean and direct chemical reduction method. The effects of initial solution pH on the sizes and dominant facets of the platinum nanoparticles are investigated and the mechanism for different sizes and facets are examined. Electrocatalytic analyses show that the catalytic activities and stabilities of the synthesized platinum nanoparticles are related to their sizes and dominant facets, and these nanoparticles display great potential as substitutes for commercial Pt/C in the effective catalysis of ethylene glycol , methanol, and ethanol electrooxidation in alkaline medium . Among the present platinum nanoparticles, the nanoparticles synthesized in pH 3 initial conditions, with small average size and (111)-dominant facets, display the best electrocatalytic activity and stability.
研究领域:
材料科学
·
化学
·
电催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2023
·
IF 6.1
Bin Wu,Shiyu Wang,Yunjian Ma,Shuguang Yuan,Frank Hollmann,Yonghua Wang
Alcohol oxidases (AOxs) catalyze the aerobic oxidation of alcohols to the corresponding carbonyl products (aldehydes or ketones), producing only H2O2 as the byproduct. The majority of known AOxs, however, have a strong preference for small, primary alcohols, limiting their broad applicability, e.g., in the food industry. To broaden the product scope of AOxs, we performed structure-guided enzyme engineering of a methanol oxidase from Phanerochaete chrysosporium (PcAOx). The substrate preference was extended from methanol to a broad range of benzylic alcohols by modifying the substrate binding pocket. A mutant (PcAOx-EFMH) with four substitutions exhibited improved catalytic activity toward benzyl alcohols with increased conversion and kcat toward the benzyl alcohol from 11.3 to 88.9% and from 0.5 to 2.6 s–1, respectively. The molecular basis for the change of substrate selectivity was analyzed by molecular simulation.
研究领域:
生物化学
·
酶学
·
食品科学
✓ 已验证
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Anqi Zhao,Mengyun Hu,Zhengying Wu,Yong Wang,Jie Li,Yukou Du
Precisely tuning the morphology of palladium-based alloys is an effective strategy for enhancing the catalytic activity in alcohol electrooxidation. However, methods for synthesizing well-defined nanowires are often not universally applicable and tend to be relatively complex. In this study, we developed a universal method to synthesize PdM nanowires (M = Sn, Pb, Sb, Bi) using a straightforward one-pot solvothermal co-reduction technique. The electronic properties of palladium can be modified through the doping of other elements. The bimetallic synergistic effect endows PdSn nanowires (PdSn NWs) with exceptional catalytic activity in both the ethylene glycol oxidation reaction (EGOR) and the ethanol oxidation reaction (EOR). Specifically, the mass activity of PdSn nanowires in the EGOR was measured at 7.56 A mgPd⁻¹, which is 3.86 times more than that of commercial Pd/C. In the EOR, the mass activity reached 6.43 A mgPd⁻¹, demonstrating an 8.14-fold enhancement over commercial Pd/C. Furthermore, PdSn nanowires also exhibited excellent stability during stability tests. This study provides significant insights into the development of nanowires catalysts with highly efficient alcohol electro-oxidation performance.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Yuting Zhong,Yalan Hu,Han Mo,Zhirui Wu,Xin Fu,Liqun Zhou,Hongying Liu,Ling Li,Xiaoguang Liu
A wrinkled rGO modified nanorod gallium oxides (Ga 2 O 3 ) anchored PdPb nanoalloys composite (PdPb@rGO/Ga 2 O 3 ) was prepared using GO/Ga-MOF as the precursor by facile hydrothermal, calcination and reduction approach, and then applied as an electrocatalyst for alcohols electrooxidation. Electrochemical tests show that the fabricated PdPb@rGO/Ga 2 O 3 exhibits superior electrocatalytic activity and high anti-CO poisoning capability for methanol, ethanol and ethylene glycol oxidation reactions (MOR, EOR and EGOR), outperforming Pd@rGO/Ga 2 O 3 and commercial Pd/C. Specifically, the bimetallic electrocatalyst owns the highest forward peak current density of 115.84 mA cm −2 , 146.97 mA cm −2 and 226.59 mA cm −2 , which is 4.69, 5.08 and 8.38 times of Pd/C for MOR, EOR and EGOR, respectively. After 3600 s CA test, the retained current density of PdPb@rGO/Ga 2 O 3 achieves the initial 59.24%, 71.13% and 81.71% towards MOR, EOR and EGOR, respectively. The remarkable performance is attributed to the electronic effects of PdPb nanoalloys, which can improve the electronic structure of Pd d-band, while the surface decoration of Pb/PbO NPs can dramatically adsorb more oxy-species and accelerate the oxidative removal of CO (ads) . Moreover, the oxidation mechanisms of three alcohols and the removal processes of CO (ads) on the Pd surface are analyzed in detail.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fengshun Wu,Li Zeng,Lihua Zhu,Weizhen Wang,Chenghao Cao,Zhiqing Yang,Congxiao Shang,Hengqiang Ye,Zhengxiao Guo
Methanol and ethanol are liquid carriers of hydrogen, convenient and safe to store and transport, particularly of interest as mobile and marine fuels. These can be directly fed into a fuel cell to impart clean energy efficiently, only if their conversion can be cost-effectively catalyzed. In this regard, a cooperative catalyst is developed with atomic Pd species, in the form of single atoms and nanoclusters, dispersed over non-noble bi-metallic CoNi alloy nanoparticles, further supported on reduced graphene oxide (rG) (Pd@CoNi/rG). The catalyst demonstrates a methanol (ethanol) oxidation, MOR (EOR), mass activity (MA) of 1.730 (3.917) A mg −1 Pd (or Pt) , 4.55 (60.26) times greater than that of the commercial 20 wt% Pt/C and 8.65 (20.61) times higher than that of the commercial 20 wt% Pd/C, respectively. More importantly, the catalyst shows excellent stability, maintaining 83.7% (93.7%) of the initial performance after chronoamperometry (CA) for 50000 s in a solution of 1 M KOH + 1 M CH 3 OH (CH 3 CH 2 OH). It significantly out-performs other mono-/bi- metallic counterparts, e.g., Co/rG, Ni/rG, Pd/rG, CoNi/rG, Pd@Co/rG and Pd@Ni/rG, due to its unique cooperative nanostructure with synergistic effects of the different metal (Pd, Co and Ni)-related species.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Nurbiye Sawut,Ruxangul Jamal,Tursun Abdiryim,Ahmat Ali,Ayigul Kadir,Zulpikar Helil,Mariyam Niyaz,Yajun Liu
It is important to select an appropriate supporting matrix, which can probably improve the electro-catalytic activity of Pt and reduce the Pt loading. In this paper, a composite (PProDOT-2MeOH:PSS/YRFC/Pt) comprising hydroxyl‑grafted poly(3,4-propylenedioxy thiophene):polystyrene sulfonate(PProDOT-2MeOH:PSS), resorcinol-formaldehyde yolk-shell carbon sphere (YRFC) and Pt nanoparticles is fabricated as electrocatalyst for methanol and ethanol electrooxidation . The PProDOT-2MeOH:PSS is uniformly coated on the YRFC, which enhances the conjugation degree of polymer and the dispersion of Pt nanoparticles to facilitate the mass transfer during catalytic reactions . PProDOT-2MeOH:PSS/YRFC/Pt has a larger electrochemical active surface area (61.02 m 2 g −1 ) than commercial 20 wt% Pt/C (17.1 m 2 g −1 ), which is resulted from anchoring sites of S atom in PProDOT-2MeOH:PSS/YRFC. The composite displays excellent electrochemical performance for ethanol and methanol oxidation with the mass activity of 1077 mA mgPt −1 and 689 mA mgPt −1 , respectively. The composite had satisfactory anti CO tolerance from the contribution of the high conductivity of PProDOT-2MeOH:PSS and YRFC. The composite also exhibits favorable cyclic stability, due to noncovalent bonding between constituents and the yolk-shell structure. These results indicate that PProDOT-2MeOH:PSS/YRFC/Pt is a promising catalyst for direct fuel cell applications .
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
Small
·
2019
·Vol. 16
·期 4
·1904964
·
IF 10.856
Zelin Chen,Yunwei Liu,Chang Liu,Jinfeng Zhang,Yanan Chen,Wenbin Hu,Yida Deng
The development of new type electrocatalysts with promising activity and antipoisoning ability is of great importance for electrocatalysis on alcohol oxidation. In this work, Pd nanowire (PdNW)/CuO x heterogeneous catalysts with different types of Pd O Cu interfaces (Pd/amorphous or crystalline CuO x ) are prepared via a two-step hydrothermal strategy followed by an air plasma treatment. Their interface-dependent performance on methanol and ethanol oxidation reaction (MOR and EOR) is clearly observed. The as-prepared PdNW/crystalline CuO x catalyst with 17.2 at% of Cu on the PdNW surface exhibits better MOR and EOR activity and stability, compared with that of PdNW/amorphous CuO x and pristine PdNW catalysts. Significantly, both the cycling tests and the chronoamperometric measurements reveal that the PdNW/crystalline CuO x catalyst yields excellent tolerance toward the possible intermediates including formaldehyde, formic acid, potassium carbonate, and carbon monoxide generated during the MOR process. The detailed analysis of their chemical state reveals that the enhanced activity and antipoison ability of the PdNW/crystalline CuO x catalyst originates from the electron-deficient Pd δ+ active sites which gradually turn into Pd 5 O 4 species during the MOR catalysis. The Pd 5 O 4 species can likely be stabilized by moderate crystalline CuO x decorated on the surface of PdNW due to the strong Pd O Cu interaction.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yuefan Zhang,Jie Li,Cheng Wang,Dongmei Liu,Rui Yu,Changqing Ye,Yukou Du
Fabricating 2D nanomaterials with heterogeneous structure is a feasible way to improve catalytic performance owing to its large surface area and tunable electron structure. However, such a category has not been widely reported in the field of alcohol oxidation reaction (AOR). In this work, we reported a new type of heterostructure nanosheet with Ru nanoparticles decorated around the edge of PdRu nanosheets (Ru-PdRu HNSs). Particularly, strong electronic interaction and sufficient active sites attributed to the construction of heterogeneous interface, is the key to the superior electrocatalytic behavior of Ru-PdRu HNSs towards methanol oxidation reaction (MOR), ethylene glycol oxidation reaction (EGOR), and glycerol oxidation reaction (GOR). Remarkably, owing to the enhanced electron transfer brought by the introduction of the Ru-PdRu heterogeneous interface, these novel nanosheets are highly durable. Apart from being able to maintain the highest current density after 4000 s chronoamperometry test, Ru-PdRu HNSs can be reactivated with negligible activity loss in MOR and GOR test after four consecutive i-t experiments. Impressively, in the EGOR test, after reactivation, the current density is step-wisely increased, making it one of the best AOR electrocatalysts.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Nannan Zhang,Jie Li,Wanyu Liang,Yangping Zhang,Zhengying Wu,Yukou Du
2D nanodendrites (NDs) and nanosheets (NSs) have been regarded as efficient nanocatalysts for enhancing the electrocatalytic performance due to their low coordinated sites and abundant electrocatalytic centers. Nevertheless, it remains challenging to construct advanced NDs and NSs in a single reaction system. Herein, by tuning the volume ratios of mixed solvents, the reduction and diffusion rate of Sn2+ on Pd NSs template was rationally controlled to prepare PdSn NDs and PdSn NSs. Ascribed to the open 2D nanostructure, high specific surface area, and robust synergistic effect, the as-prepared PdSn NDs and PdSn NSs exhibited distinguished electrocatalytic activities for ethylene glycol oxidation reaction (EGOR) and ethanol oxidation reaction (EOR), as well as commendable electrocatalytic durability, which were far superior to the Pd NSs and commercial Pd/C. In addition, the PdSn NDs exhibited enhanced reaction kinetics because the characteristic branch structure exposed a high density of active sites. This work may provide significant guidance for preparing excellent nanocatalysts with various morphological features by simply optimizing the content of the coexisting solvents.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Yang Fan,Pei-Fang Liu,Zi-Juan Yang,Tong-Wu Jiang,Kai-Li Yao,Ran Han,Xin-Xin Huo,Yun-Yi Xiong
Porous carbon spheres (PCSs) are prepared via a facile hydrothermal carbonization and chemical activation route with pectin as the biomass precursor. The as-obtained PCSs present a large specific surface area (2440 m 2 g −1 ), well-balanced micro/mesoporosity with narrow pore size distribution and high content of oxygen-containing functional groups. The structure features make the PCSs an ideal electrode material for electrochemical energy storage . As electrode material for supercapacitors , the PCSs exhibit a high specific capacitance, good rate capacity and cycling stability. Furthermore, the PCSs show attractive property as support material for Pt electrocatalysts . Pt nanowires (PtNWs) grown on the PCSs interconnect with each other to form a porous nanowires network structure. The three-dimensional (3D) hybrid catalyst material consisting of PtNWs network supported on PCSs exhibit superior catalytic activity and stability towards both methanol and ethanol electro-oxidation in acidic media. In addition, owing to the rich presence of surface oxygen groups on PCSs, the CO-poisoning tolerance of the supported Pt nanowires is greatly promoted.
研究领域:
材料科学
·
能源存储与转换
·
电化学催化
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2019
·Vol. 12
·期 5
·1173-1179
·
IF 8.515
Xu Yanchao,Cui Xiaoqiang,Wei Shuting,Zhang Qinghua,Gu Lin,Meng Fanqi,Fan Jinchang,Zheng Weitao
The development of highly efficient Pt-based alloy nanocatalysts is important but remains challenging for fuel cells commercialization. Here, a new class of zigzag-like platinum-zinc (Pt-Zn) alloy nanowires (NWs) with rough surface and controllable composition is reported. The merits of anisotropic one-dimensional nanostructure, stable high-index facets and coordinatively unsaturated Pt sites endow the composition-optimal Pt 94 Zn 6 NWs with a mass activity of 7.2 and 6.2 times higher than that of commercial Pt black catalysts toward methanol/ethanol oxidation, respectively. Alloying-induced d -band electron modulation and lattice strain effects weaken the adsorption strength of poisoning species, which originally enhances the catalytic activity of Pt-Zn NWs. This study provides a new perspective of Pt-Zn electrocatalysts with intrinsic mechanism for enhanced catalytic performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Mingzhi Chen,Sifan Zhang,Chenyu Zhu,Huan Zhang,Lihua Zhu,Yingliang Feng,Jiexiang Wang,Qian Yang,Bingqian Liu,Wentao Xu
MOFs (metal-organic frameworks) materials have been widely applied in sensing and catalysis, with the advantages of large surface area, numerous active sites, controllable size and morphology. Herein, we report the preparation of the caged PdZn/NC catalysts with the PdZn alloy nanoparticles on carbon doping with nitrogen owing high electrocatalytic performance by using a hydrothermal synthesis and pyrolysis strategy. The caged structure and PdZn alloy are demonstrated by a series of advanced characterization techniques. The material combines the advantages of bimetallic alloy and MOFs cage structure to realize highly efficient electrocatalytic oxidation of ethanol oxidation reactions (EOR) and methanol oxidation reactions (MOR) simultaneously. Electrochemical test results show that PdZn/NC-2 has a mass activity of 2.41 A mg −1 pd and 2.64 A mg −1 pd for methanol and ethanol oxidation, respectively, which is 12.68 times (MOR) and 14.67 times (EOR) higher than that of commercial Pd/C. This is probably attributed to the cage-like structure of PdZn/NC separating the Pd nanoclusters , resulting in high Pd dispersion. Simultaneously, the electronic property of Pd is adjusted after the formation of the complete PdZn alloy, improving the desorption of the carbon-based intermediates from the Pd active sites. This increases the CO poisoning resistance, resulting in good alcohol electrocatalytic oxidation activity and stability.
研究领域:
材料科学
·
电化学
✓ 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）