INORGANIC CHEMISTRY
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2023
·
IF 4.6
Ziqiang Wang,Pengjun Tian,Hugang Zhang,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Engineering two-dimensional (2D) metallic nanomaterials has attracted numerous research interests for oxygen reduction reaction (ORR) due to their highly exposed unsaturated metal atoms and excellent physicochemical properties. Herein, we report a CO-confined growth strategy for the synthesis of 2D PdCu bimetallene with several atomic layers for ORR. The incorporation of Cu into Pd metallene can generate strain effect and change the electronic structure, weakening the interaction between Pd and CO and suppressing the adsorption of CO. Therefore, the synthesized PdCu bimetallene exhibits remarkable catalytic performance for alkaline ORR, with mass and specific activities of 0.82 A mgPd–1 and 1.01 mA cm–2, which are 5.1 and 3.7 times those for Pt/C, respectively. Meanwhile, the PdCu bimetallene shows no decrease in ORR activity after 5000 cycles. This work highlights the design of ultrathin bimetallic 2D nanomaterials for efficient ORR electrocatalysis.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 46
·24694-24700
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IF 14.511
Hugang Zhang,Songliang Liu,Ziqiang Wang,Xinmiao Li,Kai Deng,Hongjie Yu,Xin Wang,You Xu,Hongjing Wang,Liang Wang
The rational design and engineering of high-performance and stable electrocatalysts for the borohydride oxidation reaction (BOR) is imperative for the development of direct borohydride fuel cells. In this work, we report a one-pot strategy for the self-assembly of Ni-doped hyperbranched PdCu nanocrystals (Ni–PdCu NCs) using polyethylene oxide as the structure-directing agent in the presence of bromide ions. Benefitting from the branched nanoarchitectures, high active sites, and trimetallic compositions, the as-fabricated Ni–PdCu NCs exhibit superior electrocatalytic performance to PdCu NCs and Pd/C towards the BOR in 1.0 M KOH containing 50 mM NaBH4, as well as better durability due to the higher resistance to BHx intermediates. The present work provides a facile route for the design of multi-metal electrocatalysts with a hyperbranched structure for direct borohydride fuel cells.
研究领域:
材料科学
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能源化学
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纳米技术
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
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IF 4.6
Wujian Zhang,Weijian Ge,Yiping Jin,Mingming Dang,Panpan Zhang,Wenfeng Han,Ying Li,Zongjian Liu,Haodong Tang
Loaded noble metal redispersion is an important way to solve catalyst sintering. However, how to redisperse at low temperatures or carbon-based noble catalysts is a difficult problem. In this paper, we report this phenomenon occurring on PdCu alloy catalysts, where small-sized PdCu alloys can be realized from sintered large-sized PdCu alloys on carbon supports in a CO/O 2 atmosphere. The mechanism of redispersion is elucidated by XPS, TEM and DFT calculations. The main reason for the redispersion is the formation of the PdCuOx intermediate, which can easily migrate to the nearby catalyst surface and then be reduced to smaller PdCu alloy nanoparticles. This work provides a deeper understanding of the redispersion phenomenon and provides certain applications in industry.
研究领域:
催化
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材料科学
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化学工程
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DOI
高影响因子
Journal of Physical Chemistry C
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2018
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IF 4.484
Zhen Chen,Ya-Chuan He,Jia-Hui Chen,Xian-Zhu Fu,Rong Sun,Yan-Xia Chen,Ching-Ping Wong
PdCu alloy flower-like nanocages are synthesized through corner-etched Cu2O octahedra as templates by galvanic reaction and disproportionation reaction. PdCu alloy nanocages are obtained with the molar ratio of H2PdCl4/Cu2O = 1:1, and the Pd nanoparticles are prepared with the molar ratio of H2PdCl4/Cu2O = 2:1. The PdCu alloy flower-like nanocages display the highest catalytic activity compared with Pd nanoparticles toward methanol oxidation reaction in alkaline medium, which is 2.7 times than that of commercial Pd/C. In addition, PdCu alloy nanocages also show high poison-tolerance and good stability. The superior electrocatalytic performance of PdCu flower-like nanocages may be attributed to the unique flower-like nanocage structure with high surface area and the synergic effect of Pd and Cu.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2024
·
IF 3.8
Gao Li,Liang Yuan,Fatimah Kehinde Busari,Yue Li,Zhangjie Li,Wen Xu,Yongdong Chen
Three-way catalysis represents a pivotal technology for converting automobile exhaust pollutants into non-toxic gases. Substituting some noble metals with transition metals is considered a promising way to reduce catalyst costs. Herein, we have investigated the catalytic potential of different configurations of Pd-Cu catalysts prepared by impregnation (PdCu/MA), sol-gel (PdCu-MA), impregnation with physical mixing (Pd/Cu/MA) and sol-gel with physical mixing (Pd/Cu-MA) to modify the interaction of Pd/Cu and MgAl1.82Ce0.18O4 (MA) spinel in this comparative study. The different structures in these catalysts lead to different catalytic performances. PdCu/MA exhibits the best three-way catalytic performance, which owe to the small-sized PdCu particles with high Pd2+ content (45.3%) and optimal interaction of Pd/Cu particles and MgAl1.82Ce0.18O4 support. Furthermore, comprehensive CO-DRIFTS, H2-TPR, and O2-TPD analyses discover that the metal-support interaction is beneficial to enhance the catalytic performance in three-way catalysis. Overall, we demonstrated that the interaction between PdCu bimetals and support can regulate the electronic state of Pd, thereby enhancing the use and efficiency of noble metals.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Haibo Yin,Junyang Zhang,Yunlong Wang,Xiaoguang Zhao,Yakun Qu,Yue Peng,Hexing Li,Yuning Huo,Junhua Li
Photocatalytic membrane reactor (PMR), coupling photocatalysis and membrane separation , has shown a considerable potential in foulant removal. However, the serious membrane fouling and fragile membrane stability still limit the application of current PMR systems. Here, we report a strategy that PdCu alloy deposited on TiO 2 , which is incorporated with polyvinylidene fluoride membrane, achieves high humic acid (HA) rejection efficiency (100%) with enhanced membrane permeation and anti-fouling performance. Detailed characterizations demonstrate that alloying effect of PdCu-TiO 2 plays multiple roles in improving PMR performance: (1) providing the paired Pd-Cu sites for enhancing HA adsorption and transferring electrons from Pd-Cu sites to HA to improve photocatalytic HA removal; (2) inducing the photothermal effect due to the carrier damping, which directly enhances membrane permeation. The remarkable properties of PdCu-TiO 2 membrane in PMR confirm the significance of alloying effect for treating aqueous organic pollutants .
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Zhao Jiang,Xiang Gong,Shuyi Guo,Yanxin Bai,Tao Fang
The NECZ/12H-NECZ (N-ethylcarbazole/dodecahydro-N-ethylcarbazole) system is regarded as the most potential liquid organic hydrogen carrier. However, the low activity, selectivity of NECZ and high cost of catalysts for the dehydrogenation reaction restrict its efficiency and commercial applications. In this work, a series of bimetallic Pd-M(M = Cu, Ni)/SiO 2 catalysts were prepared and employed to enhance catalytic activity and selectivity of NECZ for the 12H-NECZ dehydrogenation reaction. Pd 3 Ni 1 /SiO 2 exhibited high catalytic performance with 100% conversion, 91.1% selectivity of NECZ and 5.63 wt% hydrogen release amount at 453 K, 101.325 kPa for 8 h. The TOF (turnover frequency) of Pd 3 Ni 1 /SiO 2 is enhanced by 42.4% compared with Pd/SiO 2 . Combined with the characterization analysis, it was found that adjusting the alloying degree or the alloy phase in the PdCu and PdNi bimetallic catalysts could significantly enhance the dehydrogenation activity and selectivity, which were dependent on the component of bimetallic catalysts . This work may provide theoretical guidance for designing the efficient and low-cost bimetallic catalysts for the dehydrogenation of 12H-NECZ, which could boost the commercial applications of liquid organic hydrogen carriers.
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
Reaction Chemistry & Engineering
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2023
·
IF 3.9
Cheng Zhang,Yi Zheng,Jianfeng Li,Hongzhang Cao,Yanhui Xu,Weisheng Liu,Zhengping Dong
Selective hydrogenation of alkynol compounds to produce high value-added enols is an important reaction in the fine chemical industry. The construction of selective hydrogenation catalysts for alkynols is challenging because the alkynyl group is prone to over hydrogenation and the selectivity in the hydrogenation is always low. Herein, a simple sacrificial template strategy was designed to prepare mesoporous CeO2, on which ultrafine and highly-dispersed bimetallic PdCu nanoparticles were anchored, obtaining the PdCu@CeO2 catalyst. Introducing non-precious metallic Cu can improve the selectivity of precious metal Pd catalysts for the selective hydrogenation of alkynols through electronic and geometric modulation. The obtained PdCu@CeO2 catalyst showed high selectivity (99%) and good recyclability for the selective hydrogenation of the probe compound propynol ethoxylate under mild conditions. The PdCu@CeO2 catalyst also exhibited excellent performance in the catalytic selective hydrogenation of various substituted alkynols. Therefore, this research work provides a feasible strategy for the effective regulation of catalytic performance, which has potential application for the efficient catalytic selective hydrogenation of alkynols in the fine chemical industry.
研究领域:
催化化学
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材料科学
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精细化工
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Na Ye,Yanxin Bai,Zhao Jiang,Tao Fang
In the work, the catalytic performance and reaction mechanism of methanol oxidation reaction(MOR) are studied for the bimetallic Pd x Cu y and Pd x Ni y catalysts in alkaline solution. The results reveal that the Pd 1 Ni 1 /C and Pd 1 Cu 1 /C bimetallic catalysts exhibit high catalytic activity 4.1 and 3.9 times higher than that of the commercial Pd/C catalyst. Combined with the X-ray diffraction (XRD), High-resolution transmission electron microscopy(HRTEM) and X-ray photoelectron spectroscopy (XPS) analysis, the charge transfer between Pd and Cu(or Ni) alters the electron density of Pd and enhances the anti-CO poisoning ability, which is confirmed by DFT (Density Functional Theory) calculations. The CO binding energy is weakened on various bimetallic surfaces compared with that on Pd(111), consistent with experimental results. A linear relationship exists between the CO binding energy and the catalytic activity on the bimetallic catalysts, indicating that the CO binding energy may be the potential descriptor for MOR in alkaline media .
研究领域:
催化化学
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材料科学
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理论计算
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产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2016
·Vol. 27
·期 49
·495403
·
IF 3.573
Dengfeng Wu,Haoxiang Xu,Dapeng Cao,Adrian Fisher,Yi Gao,Daojian Cheng
In order to combine the advantages of both 0D and 1D nanostructured materials into a single catalyst, density functional theory (DFT) calculations have been used to study the PdCu alloy NP-decorated Cu nanotubes (PdCu@CuNTs). These present a significant improvement of the electrocatalytic activity of formic acid oxidation (FAO). Motivated by our theoretical work, we adopted the seed-mediated growth method to successfully synthesize the nanostructured PdCu@CuNTs. The new catalysts triple the catalytic activity for FAO, compared with commercial Pd/C. In summary, our work provides a new strategy for the DFT prediction and experimental synthesis of novel metal NP-decorated 1D nanostructures as electrocatalysts for fuel cells.
研究领域:
材料科学
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电化学
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理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Hongyuan Shang,Hui Xu,Qingyun Liu,Yukou Du
Hydrogen sulfide (H 2 S) could be directly produced in mammals and recognized as a third gasotransmitter, which are closely associated with physiological and pathological processes. However, the detailed mechanism remains unclear, mainly due to a lack of robust sensors to accurately and quantitatively detect its concentrations in biological samples. Herein, for the first time, we develop a new electrochemical sensor for the detection of H 2 S based on the chemical reaction between copper oxide (CuO and Cu 2 O) and hydrogen sulfide (including H 2 S and HS − ) at a neutral solution (pH 7.4). Interestingly, when Na 2 S exists, copper and its oxide can be converted into Cu 2 S and CuS, resulting in an increase in the oxidation peak current of Cu 2 S-CuS with the increase of Na 2 S concentration, which is a direct evidence confirming the excellent sensor for the H 2 S detection. More importantly, the linear relationship between the oxidation peak currents of Cu 2 S-CuS and Na 2 S concentration is observed from 0.4 μM to 400 μM with a low detection limit of 0.2 μM, and satisfying selectivity. The developed strategy may have a great potential for further understanding the roles that biological H 2 S plays in biological systems.
研究领域:
生物医学工程
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2018
·
IF 2.21
Jiawei Xia,Yongsheng Fu,Guangyu He,Xiaoqiang Sun,Xin Wang
A nitrogen-doped carbon black (NCB) supported PdCu alloy nanocatalyst is fabricated via a facile one-pot soft chemistry route. The PdCu nanoparticles are uniformly dispersed on the NCB surface with an average size of 3.51 nm. The PdCu/NCB catalyst exhibits superior catalytic activity and significantly improved durability towards the Suzuki-Miyaura coupling reaction in ethanol/water system under mild conditions without a protective atmosphere . Particularly, the Pd5Cu5/NCB catalyst can efficiently catalyzed the SMC reaction with the yield up to 94% in 1.5 h, 7-fold higher than that by the pristine Pd/NCB catalyst (13%). Compared with the carbon black supported PdCu catalyst, nitrogen-doping can lead to better dispersion of the PdCu alloy nanoparticles on the NCB surface with a smaller particle size. The excellent catalytic performance can be attributed to the unique nanostructure of the catalyst and concerted effect of the individual components. Notably, alloying Pd with Cu can effectively reduce the cost of the catalyst.
研究领域:
材料科学
·
催化化学
✓ 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）