Journal of Physical Chemistry C
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2021
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IF 4.126
Hanxue Yan,Wenbo Gao,Qianru Wang,Yeqin Guan,Sheng Feng,Han Wu,Qing Guo,Hujun Cao,Jianping Guo,Ping Chen
Palladium (Pd) has long been known to be inactive for dinitrogen activation and hence has received little attention for ammonia synthesis. Herein, we report that the reactivity of Pd is changed when reacting with lithium hydride (LiH) forming a series of lithium palladium hydrides such as LiPdH0.7 and Li2PdH2 (denoted as [Li–Pd–H]). LiPdH0.7 promotes N2 fixation by LiH forming Li2NH and LiPd, and the subsequent hydrogenation of Li2NH and LiPd leads to ammonia and regeneration of LiH and [Li–Pd–H]. Based on these experimental results, an ammonia loop mediated by a [Li–Pd–H]–LiH and LiPd–Li2NH composite pair is proposed and demonstrated. An ammonia production rate of 693 μmolNH3 g–1 h–1 was achieved at 300 °C and 1 bar, which is ca. 7 times that of the neat LiH/Li2NH pair at 350 °C and 1 bar and 2 times that of the thermocatalytic process catalyzed by Ru/MgO at 300 °C and 10 bar.
研究领域:
化学
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催化
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材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Longqiao Ran,Yongming Sui,Wenhui Wang,Fuxin Wang,Dezhou Zheng,Qi Feng,Ruijing Fu,Guangxia Wang
Direct ethanol fuel cells (DEFCs) provide a portable and environmentally friendly power source with high energy density. However, the slow kinetic of the ethanol oxidation reaction (EOR) has hindered the commercialization of DEFCs. Palladium (Pd)-based nanomaterials are the best promising catalysts for EOR due to the high catalytic activities and relatively abundant reserves. In this paper, we developed a simple and green way for the preparation of palladium hydride (PdH 0.43 ) and Au/PdH 0.43 heterostructures. Ethylene glycol (EG) provided the source of H atoms for the formation of PdH 0.43 in synthesis process. The as-synthesized PdH 0.43 and Au/PdH 0.43 nanocrystals were extremely stable under ambient conditions and annealing at 300 °C under Ar. Compared with PdH 0.43 and commercial Pd/C, Au/PdH 0.43 presented a higher mass activity of 2659 mA mg −1 , a lower oxidation peak potential, and a higher catalytic stability for oxidizing ethanol. Remarkably, the improved catalytic performance might arise from the synergistically modulation of electronic structure, the enhanced resistance to poisoning products and the acceleration of electron transfer by the formation of palladium hydrides and abundant heterostructures of Au/PdH 0.43 . This work provides a promising reference for the development of metal-hydride nanomaterials and heterostructures as efficient catalysts.
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Hui-Ying Sun,Yu Ding,Ya-Qi Yue,Qi Xue,Fu-Min Li,Jia-Xing Jiang,Pei Chen,Yu Chen
The rational design of advanced electrocatalysts and energy-saving electrolysis strategies is highly desirable for achieving high-efficiency electrochemical H2 generation yet challenging. In this work, we report highly branched Pd hydride nanodendrites (PdH-NDs) formed by a very facial solvothermal method and a succedent chemical H intercalation method in N,N-dimethylformamide. The electrocatalytic performance of PdH-NDs is experimentally and theoretically correlated with the morphology and composition, which has demonstrated substantially enhanced electrochemical activity and stability for formate oxidation reaction and hydrogen evolution reaction in alkaline electrolyte compared with Pd nanodendrites. Density functional theory calculations suggest a downshift of the Pd d-band center of PdH-NDs due to the dominant Pd–H ligand effects that weaken the binding energies of the intermediate catalytic species and toxic carbon monoxide. The asymmetric formate electrolyzer based on bifunctional PdH-ND electrocatalysts is first constructed, which only requires a low voltage of 0.54 V at 10 mA cm–2 for continuous H2 generation. This study reveals significant insights about the morphology/composition-performance relationship for palladium hydrides with bifunctional electroactivity.
研究领域:
材料科学
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电化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
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2021
·Vol. 50
·期 30
·10359-10364
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IF 4.39
Xiaoyun Guo,Zheng Hu,Jianxin Lv,Jianqiang Qu,Shi Hu
Nobel metal catalysts with high-index facets feature a high density of steps and kink sites, which bring about high activity but could be unstable during the electrocatalytic process. Doping with interstitial hydrogen atoms is a unique and effective way to regulate the electronic structure of the host materials. The formation of hydride also helps to stabilize the active sites on the surface of catalysts. Herein, we demonstrate the conformal doping of H atoms into the Pd nanostructure with preferential exposure of {730} facets, forming concave nanocubes of palladium hydride. Compared to the palladium counterparts, the palladium hydride catalysts show enhanced activity and stability in electrocatalytic methanol oxidation, and the structural differences between the Pd and PdH catalysts are revealed by XRD and X-ray photoelectron spectroscopy. Our work presents a powerful strategy for designing durable catalysts with high performance by combining high-index facet with interstitial atom doping.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2021
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IF 8.067
Yunwei Liu,Zelin Chen,Chang Liu,Jinfeng Zhang,Wenbin Hu,Yida Deng
We have developed an efficient strategy to synthesize an active and durable electrocatalyst of Pd hydride nanocubes (NCs). Instead of the traditional chemical method, the PdH 0.43 NCs are firstly prepared via a hydrogen diffusion procedure, followed by hydrothermal synthesis of an amorphous CuO layer encapsulating the PdH 0.43 NCs to prevent the hydrogen atoms from escaping. Obvious lattice expansion is demonstrated playing a pivotal role in the enhancement of their oxygen reduction reaction (ORR) activity and durability. The obtained PdH 0.43 @CuO NCs catalysts exhibit an ORR mass activity of 0.18 A mg −1 at 0.90 V versus reversible hydrogen electrode in an alkaline medium, which is about five times higher than that of commercial Pt/C. Accelerated durability tests show that there is only a 32 mV decay in half-wave potential even after 10,000 potential cycles, indicating the excellent stability of PdH 0.43 @CuO NCs. Density functional theory (DFT) calculations also indicate that, compared to Pd, PdH 0.43 has a lower limiting barrier to form OH − during the ORR process. The present study illustrates the importance of lattice expansion caused by hydrogen and offers an available strategy to design highly efficient and durable Pd-based electrocatalysts for alkaline fuel cells.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Pharmacology
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2025
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IF 4.8
Qing Wang,Daixing Zhang,Yining Qi,Changbao Huang,Dejun Ding,Chuanliang Liu
Introduction: The growing threat of bacterial infections poses a critical challenge to public health, underscoring the urgent need for innovative antibacterial agents and therapeutic strategies. In response, we have developed a multifunctional nanoplatform based on palladium-hydride metal–organic frameworks (P(H)ZPAg) for synergistic hydrogen and photothermal antibacterial therapy.Methods: This nanoplatform integrates palladium hydride (PdH) encapsulated within a zeolitic imidazolate framework (ZIF-8), surface modification with polydopamine (PDA), and in situ generation of silver nanoparticles (Ag NPs) to achieve enhanced antibacterial efficacy. Comprehensive characterization was performed to assess hydrogen release kinetics, photothermal performance, and silver-mediated bactericidal activity. The therapeutic potential of P(H)ZPAg was further evaluated in vivo using a Staphylococcus aureus-infected rat wound model.Results: The P(H)ZPAg nanoplatform demonstrated a successful combination of hydrogen release, photothermal conversion, and silver ion-based antibacterial mechanisms. In vitro assays revealed potent synergistic antibacterial effects against both Escherichia coli and Staphylococcus aureus. In vivo studies showed that treatment with P(H)ZPAg nanoparticles significantly enhanced wound healing and bacterial clearance compared to control groups.Discussion: These findings highlight the potential of combining hydrogen therapy, photothermal therapy, and silver ion release within a single nanoplatform to markedly improve antibacterial outcomes. This study presents a promising strategy for the development of multifunctional nanotherapeutics, offering a novel and effective approach for managing topical bacterial infections and promoting wound healing.
研究领域:
生物医学工程
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纳米医学
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感染与免疫
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产品关联
DOI
PubMed
高影响因子
Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Qiu Yu,Jiao Dongxu,Huang Hong,Wu Jiandong,Wang Mingming,Gao Tianyi,Zhao Xiao,Ge Xin,Zhang Wei,Zheng Weitao,Singh David J.,Fan Jinchang,Cui Xiaoqiang
Palladium hydride (PdH x ) metallenes are efficient electrocatalysts for the oxygen reduction reaction (ORR) due to their high atomic utilization and optimized oxygen binding energies modulated by interstitial hydrogen. However, their practical application is restricted by the highly unstable nature of interstitial hydrogen at working temperatures around 353 K. Here, we report that the use of Mn effectively locks hydrogen atoms within the Pd metallenes lattice, resulting in high alkaline ORR performance across a temperature range of 303–353 K. In contrast, the ORR activity of PdH x metallenes declines sharply with increasing temperature. At 353 K, the mass activity of PdMnH x metallenes at 0.95 V reaches 1.41 A mg − 1 , which is 14.1 times higher than that of PdH x metallenes. Multiple spectroscopic analyses and theoretical calculations reveal that strong electronic interactions within the immiscible Pd-Mn alloy are critical for locking interstitial hydrogen, thereby enhancing the ORR activity under high temperatures.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Wang Hengjia,Qin Ying,Wu Yu,Qiu Yiwei,Ling Ling,Fang Qie,Wang Canglong,Hu Liuyong,Gu Wenling,Zhu Chengzhou
Hydrogen adsorption and desorption in single-phase catalysts often occur at a single catalytic site based on the traditional hydrogen evolution reaction (HER) pathway, which makes it difficult to break the limitation entailed by the Sabatier principle. Herein, β-Pd hydride metallene (β-PdHene) aerogels are synthesized as advanced HER catalysts. A lattice hydrogen-involved mechanism is reported to separate adsorption and desorption sites, which is thermodynamically favorable compared to the traditional reaction pathway. In situ differential electrochemical mass spectrometry and theoretical calculations reveal that lattice hydrogen as additional active sites directly participate in the HER process. Consequently, β-PdHene aerogels exhibit a low overpotential of only 20 mV at 10 mA cm −2 and remarkable HER stability, which are even comparable to commercial Pt/C. Our work opens an avenue to rationally develop highly active HER catalysts, bypassing the design limitations of catalysts under traditional mechanisms.
研究领域:
材料科学
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化学工程
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催化
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电化学
✓ 已验证
DOI
高影响因子
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