NANOTECHNOLOGY
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2022
·Vol. 33
·期 38
·385703
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IF 3.953
Mei Zhang,Lin Cui,Qiqi Mao,Ziqiang Wang,Hongjie Yu,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Exploring cost-effective and highly active electrocatalysts is of great significance for sustainable electrochemical NH3 synthesis. Palladium (Pd)-based catalysts have been unanimously considered as one of the most efficient catalysts for the nitrogen reduction reaction (NRR). Herein, self-supported mesoporous Pd film with partial oxidation on Ni foam (mPd-PdO/NF) was synthesized through the micelle-assisted chemical replacement method coupled with air oxidation under 260 °C, and the mPd-PdO/NF electrocatalyst exhibited superior NRR performance with the maximum values of rNH3 (24.8 mg h−1 mgcat.−1) and FE (16.64%) were obtained at −0.1 V, relative to the single counterparts (mPd/NF and mPdO/NF). It is proposed that both metallic Pd and its oxide domains when co-existing with a phase boundary between them can facilitate nitrogen activation and hydrogenation, resulting in an enhanced NRR performance. This work provides an inspiring strategy for the rational design of highly active and durable metal–metal–oxide nanoarchitectonics for ammonia electrosynthesis.
研究领域:
电化学
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材料科学
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催化
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可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Lulu Kong,DeZhu Chen,Xiaolong Zhang,Lin Zhou,Yongming Deng,Shaohua Wei
The growth of oxides on the surface of noble metals and the introduction of alloys are effective methods to enhance the catalytic activity of noble metals. However, the fabrication of noble metal oxides always involves harsh experimental conditions and the oxidation degree could not be controlled. Herein, a simple, fast, and controlled Pd oxidation method by mixing Hg2+ and Pd nanosheets (PdNSs) under mild conditions to form PdxHgy(PdO)z (PHOs) was reported, which consists of the Pd–Hg alloy and PdO. The density functional theory (DFT) calculation and experiment results proved that the Hg atom incorporation promotes the nearby Pd–Pd bond breaking, initiating a cascade of PdO generation. More precisely, 1 Hg atom incorporation induced ∼8 Pd atom oxidation, ensuring that the oxidation degree of Pd could be easily controlled by adjusting the ratio of Hg2+ and PdNS. As a peroxidase-mimicking nanozyme, the PHO affinity for its substrate could be 21.7- and 123.6-fold greater than that of the PdNS and the natural peroxidase (HRP), respectively. For the colorimetric immunoassay of carcinoembryonic antigen (CEA) detection, PHO has an ultralow detection limit of 1.33 pg mL–1, which is ∼8.6 and ∼282 times lower than that of the PdNS and the natural HRP, respectively.
研究领域:
生物化学
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医学诊断
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2019
·Vol. 95
·期 3
·862-874
·
IF 2.659
Fei Rao,Gangqiang Zhu,Miaomiao Wang,Siyaka Mj Zubairu,Jianhong Peng,Jianzhi Gao,Mirabbos Hojamberdiev
BACKGROUND Photocatalysis is one of the effective ways to solve the problem of water and gas pollution. An excellent photocatalyst should have the following advantages: efficient photocatalytic activity for gas and water pollutants, recyclable and stable characteristics, non-toxic and low-cost. Constructing heterojunctions and introducing oxygen vacancies (OVs) are two effective measures to achieve these targets. RESULTS It is found that the 1.0% Pd/PdO/β-Bi 2 O 3 exhibits the best photocatalytic activity with an efficiency of 97.4% for Bisphenol A (BPA) degradation and 47.6% for nitric oxide (NO) removal within 30 min. The 1.0% Pd/PdO/β-Bi 2 O 3 composite shows 23.3% efficiency in the photodegradation of BPA under 595 nm monochromatic light irradiation, while β-Bi 2 O 3 tends to be invalid. Moreover, the OVs promote the removal of NO without irradiation. CONCLUSION In this work, a novel ternary Pd/PdO/β-Bi 2 O 3 material as high-performance photocatalyst for the BPA degradation and NO removal was synthesized. The presence of OVs promotes the activation of the oxygen molecule, thereby facilitating the photocatalytic process. The p - n junction of PdO/β-Bi 2 O 3 and the Schottky barrier of Pd/β-Bi 2 O 3 significantly limit the recombination of photoinduced electron–hole pairs in the composite. Furthermore, an artifact in the electron spin resonance (ESR) spectrum obtained by spin trapping with 5,5-dimethyl-1-pyrroline N -oxide (DMPO) as adducts confirms that both hydroxyl radical (•OH) and superoxide radical (•O 2 − ) species are involved in the photocatalytic process. The present work offers a new perspective for developing the composite photocatalysts with high efficiency through loading of metal nanoparticles and creating an heterojunction. © 2019 Society of Chemical Industry
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 3
·325
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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
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材料科学
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化学工程
✓ 已验证
产品关联
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
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化学传感器
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yuan Zhou,Xun Zhu,Biao Zhang,Ding-Ding Ye,Rong Chen,Qiang Liao
Formic acid as a renewable fuel can be converted to clean electricity in fuel cells by high-efficient electrochemical oxidation . The conversion rate is fundamentally dictated by the synergy of interactive aspects: catalytic activity , accessibility to active sites, electron transfer , and anti-poisoning stability. For the first time, ordered mesoporous carbon (OMC) is used as the substrate for Pd–PdO catalyst for fuel cells. The unique ordered pore-channel network of OMC can enhance the spatial dispersion of Pd nanoparticles on the pore-channel wall, while the hollow pore-channel can facilitate reactant transport. Microwave and annealing treatments are found to enhance the chemical reduction and to strengthen the anchoring of Pd–PdO catalyst on OMC substrate, respectively. The OMC supported Pd–PdO catalyst (Pd–PdO/OMC) shows 1.7-fold and an order of magnitude higher mass activity and stability as compared to commercial Pd/C catalyst. For fuel cell testing, the Pd–PdO/OMC catalyst is applied to an air-breathing microfluidic fuel cell and achieves a maximum power density of 63.0 mW cm −2 , at least one-fold higher than similar previous reports.
研究领域:
材料科学
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能源科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2014
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IF 6.007
Xingfa Li,Xin Liu,Lili Xu,Yuezhong Wen,Jianqing Ma,Zucheng Wu
Heterogeneous Pd catalytic Fenton-like systems with in-situ-generated H 2 O 2 have recently gained significant attention for wastewater treatment. Intense research efforts have been focused on developing highly efficient Fenton-like catalysts. It is known that nanoparticle size and appropriate coordination of active compositions are important for the fabrication of a highly efficient multicomponent catalyst. Unfortunately, effects of these factors on Fenton-like reaction are still unknown. To decipher the puzzle, we designed multicomponent Pd/PdO/Fe 2 O 3 nanoparticles in SBA-15 (denoted as FePd-SBA) as a Fenton-like catalyst which possesses uniform and highly dispersed nanoparticles (small size about 5 nm) in space-confined channels of SBA-15. The fabricated catalyst shows high catalytic activities in Fenton-like reaction for dye degradation. For example, 98.6% removal of dye Acid Red 73 was obtained under in-situ generation of hydrogen peroxide. In contrast, when the catalyst loaded on SiO 2 without channels or pores (FePd–SiO 2 ) was prepared, and compared with FePd–SBA, FePd–SiO 2 showed noticeably poor performance (51.6%) under same conditions. Obviously, such a difference in results is due to the confinement effect of SBA-15 porous channels. It was also found that Fe and Pd played important roles in the synergistic effect, that is, Pd worked in in-situ H 2 O 2 generation and Fe species worked in decompose H 2 O 2 to degrade organic pollutants. When we applied this catalyst for Fenton-like reaction with addition of H 2 O 2 , it was also found that Pd and PdO played important roles and the synergistic effect between Fe and Pd species actually existed in dye removal. The unique nanostructure makes the catalyst to be a novel and welcoming choice for H 2 O 2 favorite reactions.
研究领域:
环境科学
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催化化学
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材料科学
✓ 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）