JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Lingling Li,Yingliang Feng,An Pei,Lihua Zhu,Weizhen Wang,Guang Li,Chengxiu Huang,Zhiqing Yang,Hengqiang Ye
Different atomic ratios of PtPd alloy nanoparticles (NPs) supported on carbon doping with nitrogen-NC (Pt x Pd y /NC) are successfully prepared to simultaneously enhance hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR), in which Pt 5 Pd 5 /NC with an atomic ratio of 5:5 has the best performance. Pt 5 Pd 5 /NC exhibits a significantly reduced HER overpotential (12 mV@10 mA cm −2 ) and the mass activity (MA) for MOR is up to 6.85 A mg −1 PtPd , 11.61 and 34.25 times higher than that of commercial Pt/C (Pt/C-JM) and commercial Pd/C (Pd/C-JM), respectively. Remarkably, coupling boosted HER on the cathode with accelerated MOR on the anode, efficient H 2 generation is achieved. This two-electrode flow cell only requires a cell voltage of 1.100 V at 100 mA cm −2 and can be stably operated for >300 h at 1.960 V with impressive long-life stability. Such performance even outperforms that of (IrO 2 ) OER‖HER (Pt/C-JM) cell. Electrochemical in-situ Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) analysis show that electronic effect is formed between N and PtPd and can oxidize the intermediate HCOO - at a lower potential (0.300 V), promote the desorption of the toxic intermediates and improve the catalytic property.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Fengyu Zhang,Yanping Yang,Qian Wang,Xiaomeng Chen,Lulu Xie,Xintao Li,Dianqing Li,Junting Feng,Xue Duan
When single-atom catalysts are oriented toward practical applications, in addition to balancing the seesaw between activity and selectivity, the capability of thermal management also merits attention. Herein, we proposed a facility approach that, based on active Pd in the state of a single atom, tunes the guest Cu size to simultaneously enhance the effect of d-electron domination and the heat transfer behavior in microregions. Along with the Cu size in an order of magnitude increase, more delocalized electrons were generated and transferred to isolated Pd sites, with the d band center shifting from 1.438 to 1.052 eV, closer to the Fermi level. Simultaneously, more long-range ordered lattices are much favorable for transferring in situ generated thermally phonons with the diffusivity surging from 12.36 to 103.49 mm2/s. The optimized Pd1Cu-SAA catalyst exhibited state-of-the-art performance in acetylene hydrogenation, achieving full conversion at 140 °C, with 95.3% selectivity and good stability in the test period.
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
PubMed
高影响因子
ChemSusChem
·
2025
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IF 6.6
Qian Jiang,Zuzhi Li,Javier Remón,Hui Xin,Zhicheng Jiang,Bi Shi
Finding new catalytic applications for tannin, a biomass resource, exploiting its structural features and renewable nature, helps contribute toward carbon neutrality in catalysis. In this study, novel Pd-supported, carbon-neutral catalysts have been synthesized using tannic acid. First, tannic acid was cross-linked and coated on the surface of nano-SiO2. This material was then subjected to controllable carbonization, with the temperature being optimized, to obtain the catalyst support SiO2@TA-T (T: carbonization temperature). Experimental results demonstrated that carbonizing at 400 °C remained part of the phenolic hydroxyls of tannin with satisfactory reducing ability. Meanwhile, the condensation and the deoxygenation of tannin increased the thermal stability of this support and introduced porous structures and abundant defect sites. This material was then used to adsorb and in situ reduce Pd2+ to develop Pd-based catalysts. To this end, this synthesized Pd/SiO2@TA-400 catalyst was then used to hydrogenate vanillin, with a conversion of 99% to vanillyl alcohol at a pressure of 0.5 MPa initial H2 and a temperature of 20°C for 60 min. Such remarkable results were corroborated in the hydrogenation of several lignin-derived aromatic aldehydes, with our catalyst achieving high conversion and outstanding recyclability (5 recycles).
研究领域:
催化化学
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生物质利用
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环境科学
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产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 8
·2519-2530
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IF 6.177
Lixue Qi,Jiajun Dai,Yichen Liao,Jian Tian,Daohua Sun
The low olefin selectivity of Pd-based catalysts is a long-term challenge for the selective hydrogenation of 1,3-butadiene. Hybrid Pd/metal–organic framework (MOF) catalysts may help tackle this problem as they can stabilize Pd nanoparticles and regulate their electronic property. Herein, both surface-supported Pd/ZIF-67 and encapsulated Pd@ZIF-67 catalysts were prepared to explore the synergy between Pd and ZIF-67 and the structure–performance relationship of the catalysts. SEM and TEM reveal the different spatial positions of Pd on the two catalysts. Interestingly, encapsulated Pd@ZIF-67 shows excellent catalytic performance in the 40 h test, with a conversion of 100% and a butene selectivity of 98%, outperforming the surface-supported Pd/ZIF-67 catalyst. XPS, CO-IR and DFT calculations indicate that the encapsulated structure promotes the synergistic interaction between the ZIF-67 and Pd sites. Furthermore, in situ DRIFTS of 1-butene reveals that the enhanced synergistic interaction weakens the adsorption of 1-butene on the catalyst surface while inhibiting its isomerization and further hydrogenation. The presented strategy together with the mechanistic results clarify the relationship between the structure and the synergistic interaction and provide a promising approach for the application of synergistic interactions in hydrogenation catalysts.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Junyu Wang,Jiangnan Guo,Qinggang Zhou,Yuejin Zhu,Qizhi Liu,Shuozhen Hu,Xinsheng Zhang
Formic acid is a desirable liquid hydrogen storage compound for solving transport and storage problems of hydrogen for onboard fuel cells. Optimizing adsorption/desorption energy of intermediates can directly modulate the performance of Pd catalysts in formic acid dehydrogenation (FAD). Herein, we introduce internal electric field with controllable strength to regulate the adsorption/desorption of intermediates on Pd. Non-ferroelectric cubic-phase barium titanate (CBT) is heat-treated at high temperature to obtain ferroelectric tetragonal-phase barium titanate (TBT(C)), which exhibits internal electric field. The strength of the internal electric field is successfully adjusted by heat treatment at different temperatures. The size of Pd nanoparticles is restricted between 2.2 and 2.7 nm, and the electronic effect of Pd is effectively eliminated by coating TBT(C) with mesoporous carbon shell (TBT(C)@SC). Experimental results prove that the internal electric field promotes the desorption of hydrogen on Pd. Pd/TBT(C)@SC-800 obtained by heat treatment at 800 °C, with the optimal internal electric field strength, exhibits high activity and hydrogen selectivity for FAD. This work provides a new strategy for designing FAD catalysts.
研究领域:
化学
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
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2024
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IF 5.2
Peng Bai,Yicheng Zhao,Yongdan Li
Photocatalytic N -formylation of amines with CO 2 is a promising strategy to convert CO 2 into value-added chemicals sustainably. In this work, Pd-Bi bimetallic modified ZnO enriched in oxygen vacancies is constructed for photocatalytic CO 2 formylation of benzylamine at room temperature without any reductants. The Pd and Bi sites reduce the band gap energy of ZnO, promote the separation of the photogenerated charge carriers and enhance the adsorption capacity of CO 2 . The yield of N -benzylformamide reaches 31.7 mmol g −1 with a selectivity of 85.3 % after 3-hour radiation in N , N -dimethylformamide (DMF) solvent. The aldehyde group involved in the formylation of benzylamine is derived from the decomposition of DMF, which is regenerated with the aldehyde group coming from the reduction of CO 2 . The decomposition-regeneration cycle of DMF solvent enlarges the reaction region, which is beneficial to the activity and selectivity of the formylation process. The synergistic photocatalytic system shows a good universality. This study provides a new approach to high-efficiency CO 2 utilization and formamide production.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Wei Jia,Wengang Liu,Yuandong Cui,Hang Song,Chengfeng Zhou,Wei Jiang,Haoxi Ben,Xiaoli Yang,De Chen
Converting cellulose into C 2 alcohols presents a sustainable alternative to fossil fuels, contributing to the development of eco-friendly and economically viable biofuels and chemicals. Tungsten oxide (WO 3 ) is a key solid acid catalyst for this process, yet limited research explores its diverse morphologies and unique catalytic effects. This study investigates diverse WO 3 morphologies (nanosheets, nanoflowers, nanoblocks, and tetrahedral octahedra) in combination with Pd for converting cellulose to C 2 alcohols. Optimized conditions with Pd/o-WO 3 catalyst resulted in the highest C 2 alcohols (ethylene glycol and ethanol, 80.9 %), notably yielding 64.8 % ethylene glycol. Extensive characterizations and DFT calculations reveal the smaller element occupancy rates and a longer W-O bond length led to a large number of crystal defects over Pd/o-WO 3 . It facilitated the formation of W 5+ –OH sites and Pd-O(H)-W interactions, further synergistically enhancing hydrogenation ability and acidity. Designed experiments to elucidate cellulose conversion pathways, including hydrolysis, retro -aldol condensation, and hydrogenation. This study emphasizes the unique impact of WO 3 morphologies and underscores the importance of supporting crystal defects for catalytic performance in eco-friendly biofuel and chemical production.
研究领域:
催化化学
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可再生资源与环境科学
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产品关联
DOI
高影响因子
FUEL
·
2024
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IF 6.7
Hong Wang,Zhongming Wang,Zizhong Zhang,Yaming Fan,Xianzhi Fu,Wenxin Dai
A prepared p-type PdO/n-type TiO 2 junction was prepared as the catalyst for photocatalytic hydrogen evolution from formic acid (FA). It was found that PdO/TiO 2 exhibited 1298-fold higher activity than TiO 2 under ultraviolet and visible light irradiation at room temperature. Multiple characterization techniques were utilized to demonstrate that doping PdO into TiO 2 can regulate the Fermi level of the sample and the adsorption behavior of FA, resulting in different electron transfer behavior between FA and PdO/TiO 2 compared to that between FA and TiO 2 . Oxygen vacancies acted as electron donors to deliver photogenerated electrons from TiO 2 to the adsorbed bidentate FA, which increased the electron density on the O atom of FA and led to the formation of activated monodentate FA. This activated FA was more easily oxidized by the holes in PdO generated by visible light, leading to the production of H 2 and CO 2 . The mode of adsorption associated with the Pd 2+ site is the key factor in driving this reaction and leading to the reversible electron transfer phenomenon. This study provides a new promising route for the design of photocatalysts for self-decomposition reactions.
研究领域:
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
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Junjing Li,Han Yu,Yongjiao Ding,Liang Wang
In order to improve the metal utilization of the noble metal Pd and the catalytic activity of the reaction, a novel and efficient Pd/Ti 4 O 7 /Ti electrode was prepared by introducing a Ti 4 O 7 intermediate layer for electrocatalytic hydrodechlorination (EHDC) of chlorinated pharmaceuticals and personal care products (PPCPs). The presence of oxygen vacancies (Ov) on the Ti 4 O 7 surface was confirmed by electron paramagnetic resonance (EPR). The results showed that the introduction of Ti 4 O 7 increased the electrochemical active surface area electrode (ECSA) of the Pd/Ti 4 O 7 /Ti electrode, accelerated the electron transfer rate on the catalyst surface, and promoted the generation of electron-rich Pd, which in turn improved the dechlorination efficiency. The Pd/Ti 4 O 7 /Ti electrode had a removal efficiency of 99.6% for florfenicol (FLO) within 180 min. Meanwhile, the removal efficiency of the Pd/Ti 4 O 7 /Ti electrode was still above 95% in seven cycles, which significantly improved the catalytic activity and stability compared with that of the Pd/Ti electrode. In addition, the reaction pathway for the electrocatalytic hydrodechlorination process of FLO at Pd/Ti 4 O 7 /Ti electrode was proposed. The ecotoxicity of the pollutants was also evaluated by the Toxicity Estimation Software Tool (T.E.S.T) model. In this study, an efficient electrocatalyst for EHDC was explored, and the Pd/Ti 4 O 7 /Ti electrode provided strong support for pollutant removal.
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
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shuchao Jiang,Hongqi Shi,Yuzhe Xu,Jiaojiao Liu,Tie Yu,Guoqing Ren
Formic acid (FA, HCOOH) is regarded as one of the most promising carriers for hydrogen storage. However, the catalyst design for FA dehydrogenation into H2 with high efficiency is not clear. Here, we elucidate the rationale of size effect over the most commonly used Pd-based catalyst through supporting different Pd species, including single atoms, nanoclusters, and nanoparticles, on amine-functionalized active carbon (Pd/AC-NH2). The activity test presents that Pd/AC-NH2 with Pd nanoclusters exhibits the best turnover frequency (TOF) value of 40856 h–1 for 1 M FA at 328 K and even 1504 h–1 for neat FA at 308 K, which is comparable to the homogeneous catalysts and has been the first heterogeneous catalyst used in neat FA dehydrogenation under mild conditions. The comprehensive characterizations reveal that the size of Pd species affects the ratios of Pd0/Pd2+ and hydrogen spillover effect, which is crucial for the C–H cleavage and H2 desorption. Besides, the influences of amine groups on catalytic performance were further examined. This work provided an ingenious guideline to design efficient and practical catalysts for hydrogen storage under ambient conditions.
研究领域:
化学工程
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材料科学
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能源科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Guanghui Yang,Hugang Zhang,Jiarong Li,Yile Wang,Kai Deng,Hongjie Yu,Hongjing Wang,Ziqiang Wang,Liang Wang
It is important to achieve sustainable ammonia production under mild conditions, and the electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy. However, the precise construction of highly active NRR electrocatalysts for ammonia synthesis remains challenging. Here, we construct B-doped PdRh mesoporous nanotubes (B-PdRh MNTs) as efficient NRR electrocatalysts. The mesoporous nanotubular structure provides abundant active sites, and B doping enhances the adsorption energy of N2. As such, the NH3 yield and Faraday efficiency of B-PdRh MNTs reach 12.03 μg h–1 mgcat–1 and 16.28% under 0.1 M Na2SO4, respectively. This work provides strategies for B-doped catalysts for efficient electrocatalytic NRR applications.
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
JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Lina Guo,Ligang Yan,Ruijun Xie,Limin Han,Ning Zhu
In this work, we investigate a palladium complex exhibiting aggregation-induced emission enhancement (AIEE) properties and remarkable solvatochromism behavior driven by structural changes arising from solvent-solute interactions. Specifically, in polar aprotic solvents, the color of the Pd complex changes from blue to purple as solvent polarity increases, accompanied by a blue shift in the UV–Vis spectrum. Notably, this blue shift is even more pronounced in polar protic solvents, which also show a significant increase in fluorescence emission. These effects are likely driven by hydrogen-bond interaction between the protic solvents and the Pd complex. Density Functional Theory (DFT) calculations show that increased solvent polarity significantly alters the electronic distribution of the Pd complex. Higher solvent polarity leads to a higher orbital transition energy, resulting in a blue shift in the UV–Vis absorption spectrum. X-ray single-crystal structure analysis further reveals that hydrogen-bonding interactions between the Pd complex and methanol stabilize its planar structure. When water is introduced, the Pd complex undergoes aggregation through non-covalent interactions, which modify the stacking arrangement. This change weakens the π-π interactions between adjacent molecules, thereby minimizing energy loss in the system. Consequently, the Pd complex effectively utilizes the AIEE mechanism to detect water content in methanol.
研究领域:
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）