ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Luyao Li,Rundong Wu,Jianhua Guo,Mengrong Han,Shiji Guo,Weiping Chen,Gang Feng,Xinwu Ba,Xin Wen
Furfural-based bifuran diacids/diesters, such as 2,2′-bifuran-5,5′-dicarboxylic acid (BFDCA), are important biomass-derived chemicals in the production of high-performance polymers and plasticizers. However, the synthesis of bifuran diacids/diesters lacks an efficient heterogeneous catalytic system. Here, we report that the interstitial modification of a PdNi bimetallic nanoalloy with boron atoms supported on nitrogen-doped carbon exhibited high catalytic efficiency in the conversion of halogenated furoic acids/esters to bifuran diacids/diesters via sequential oxidative addition and reductive elimination steps initiated at room temperature, affording a high yield with a Pd/Ni molar ratio of 1:1. The conversion of 5-bromo-2-furoic acid to BFDCA has a turnover frequency value of up to 672.0 h–1, 2.5 times higher than that of commercial Pd/C. The comprehensive characterization results demonstrated that boron as an interstitial atom entered into the lattice of the PdNi alloy, leading to lattice distortion and the regulation of the electronic state of Pd. Density functional theory calculations exhibited that these electronegative Pd sites were pivotal active species in the oxidation addition, where Ni facilitated the coordination of Pd and carbon–halogen bonds. The optimal catalyst showed excellent stability and recyclability in alkaline aqueous solution. This protocol provides an efficient strategy for the reductive homocoupling and sustainable production of bifuran diacids/diesters and their derivatives from biomass resources.
研究领域:
催化化学
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材料化学
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可持续化学
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生物质转化
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纳米材料
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有机合成
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DOI
高影响因子
IONICS
·
2023
·Vol. 29
·期 11
·4825-4833
·
IF 2.8
Yu Dan,Dong Seng,Liu Qian,Jia Weiyi,Gao Faming,Wang Yatao
The preparation of platinum-free electrocatalysts with ideal oxygen reduction reaction (ORR) activity is of great significance for cost-effective fuel cells. Herein, we synthesize a series of Pd-based (PdFe, PdCo, PdNi, and Pd) nanowires (PdM NWs). Their diameters are about 10 nm. And the lengths are up to even micrometers. The mass activity of the series of Pd-based catalysts followed the descending order: PdNi NWs/C > commercial Pt/C > PdCo NWs/C > PdFe NWs/C > pure Pd NWs/C. The optimal half-wave (E 1/2 ) of PdNi NWs/C (839 mV) is positive shift 138 and 25 mV compared with pure Pd NWs/C (701 mV) and commercial Pt/C (814 mV), respectively. The mass activity (MA) of PdNi NWs/C only dropped 28% after 10,000 potential cycles between 0.6 and 1.1 V versus RHE in acid medium. This work provides a promising and reliable strategy to synthesize high performance Pd-based electrocatalyst, which is promising alternative to expensive Pt-based electrocatalysts for fuel cells. Graphical Abstract TOC: We prepared bimetallic PdNi nanowires, which ORR mass activity higher than pure Pd nanowires and commercial Pt/C in acidic medium.
研究领域:
材料科学
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电化学
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能源催化
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Qi Xue,ZhiYu He,Kun Liu,Juan Bai,Yu Chen,Yuanzhen Zhou
The rational design of interfacial active sites is crucial for enhancing the activity and durability of Pd-based electrocatalysts for ethanol oxidation reaction (EOR). Herein, an ultrathin PdNi metallene (PdNiene) with unique asymmetric Pd─O─Bi oxo-bridge sites (PdNi-O-Biene) is synthesized via a multi-step hydrothermal method. The ultrathin 2D nanosheet structure of the metallene enables abundant exposure of Pd active sites. Notably, Ni incorporation facilitates OH * adsorption/formation and thereby promotes the oxidative removal of CO * intermediates, while the Bi-induced asymmetric oxo-bridge interface triggers interfacial charge redistribution around Pd active centers, which further facilitates CO * desorption/oxidative removal and efficient C─C bond cleavage, thus favoring the C1 reaction pathway. As a result, the optimized PdNi-O-Biene demonstrates exceptional mass activity (8.42 A mg Pd −1 ) and specific activity (28.09 mA cm ECSA −2 ) for EOR in alkaline electrolyte, representing improvements of 5.5 and 3.7 times over commercial Pd nanoparticles (Pd NPs), respectively. This work not only provides an effective strategy for the synthesis of high-performance EOR electrocatalysts but also highlights the potential of atomic-scale interface engineering for alcohol oxidation reactions.
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 58
·14472-14477
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IF 5.236
Hongjing Wang,Shiqian Jiao,Songliang Liu,Hugang Zhang,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Graphical The mesoporous PdNi/Ni nanoparticles assembled nanotubes (mPdNi/Ni NTs) have been synthesized via replacement reaction, in which nickel nanowires serve as sacrificial template to form tubular structure and the diblock copolymer induce the formation of mesoporous structures. Due to the mesoporous nanoparticle structure and tubular geometry, the mPdNi/Ni NTs have better catalytic performance than mesoporous Pd nanotubes and commercial Pd black for ethanol oxidation reaction. The optimization of structure and composition is essential to improve the performance of catalysts. Herein, mesoporous nanoparticles assembled PdNi/Ni nanotubes (mPdNi/Ni NTs) are successfully fabricated using nickel nanowires as sacrificial template. The combination of nanotubular structure with mesoporous nanoparticle morphology can provide facilitated transfer channels and sufficient active sites, allowing the full contact and reaction between catalysts and reactants. Therefore, the synthesized mPdNi/Ni NTs exhibite superior ethanol oxidation performance to mesoporous Pd nanotubes and commercial Pd black. This study proposes a rational strategy for the development of nanoparticle assembled nanotubes with surface mesoporous morphology, which can greatly improve catalytic performance in various electrocatalytic fields.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 36
·17771-17777
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IF 9.931
Yue Zhao,Yu Ding,Bin Qiao,Kai Zheng,Pei Liu,Fumin Li,Shuni Li,Yu Chen
Proton-coupled electrocatalytic reactions, such as the oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) in acidic media, are very important half-reactions of fuel cells and water electrolysis. Aiming at increasing the interfacial proton concentration to improve the ORR/HER activity, we synthesize PdNi alloy nanostructures (PdNi-ANSs)–polyethyleneimine (PEI) inorganic–organic nanocomposites (PdNi-ANSs@PEI) by a PEI assisted cyanogel-reduction strategy. Various physical characterization techniques show that PdNi-ANSs are successfully functionalized by the PEI polymer during the synthesis of PdNi-ANSs@PEI because of the N–Pd interaction. Thanks to the increased interfacial proton concentration caused by the protonation of amine groups at PEI in acidic media, the molecular weight optimized PdNi-ANSs@PEI exhibit enhanced ORR/HER activity compared to PdNi-ANSs without PEI and commercial electrocatalysts, which indicates that the electrocatalytic activity of metal nanostructures can be remarkably improved by reasonable interface design.
研究领域:
电化学
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材料科学
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催化反应
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2026
·
IF 6.7
Yuyang Zhang,Zixuan Chen,Yuqing Zhang,Qiong Wu,Yipu Wang,Jiaying Dong,Zihan Yuan,Jingyun Liang,Yang Wu,Zhengbo Han
The application of Pickering emulsions in interfacial catalysis provides a promising platform for biphasic reactions. Metal–organic frameworks (MOFs), owing to their high surface area, tunable porosity, and flexible functionalization, have emerged as ideal stabilizers for Pickering emulsions in such catalytic systems. Herein, we report the incorporation of PdNi alloy nanoparticles into MIL-101, where the Lewis acidity of the MOF combined with the catalytic activity of PdNi NPs enables two-step one-pot reactions. Interestingly, the resulting bimetallic PdNi@MIL-101 not only acts as an effective emulsifier to stabilize Pickering emulsions, but also exhibits superior performance in the reductive amination of Nitroarenes compared with the corresponding monometallic@MOFs. Moreover, PdNi@MIL-101 demonstrates excellent stability, maintaining high reproducibility after five consecutive cycles. This work not only reduces the catalyst cost, but also exploits the synergistic effect of bimetallic components and interfacial catalysis, which opens up new avenues for efficient and environmentally friendly organic synthesis.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jun Zhang,Xinlan Xu,Lanyu Luo,Tiantian Peng,Boyu Liu,Lingying Jiang,Meng Jin,Rong Wang,Huan Yi,Weimin Wu,Shi-Yu Lu
The selective exposure of active surfaces has garnered exceptionally widespread attention in enhancing electrocatalytic performance for oxygen reduction reactions (ORR). Nevertheless, because unmanageable growth thermodynamics and kinetics, the exposure of active surface not only hinders the formation of high-index facets but also induces irreversible reconstruction of low-index facets at high-potential region. Therefore, the controlled synthesis of Pd-based nanocrystals featuring high/low-index facets is highly desirable. In this study, bimetallic PdNi alloys with high/low-index facets were successfully synthesized through crystal structure engineering. Assisted by Ni 2+ , the transition from low-index facets to high-index facets was achieved. These structural features endow PdNi alloy nanocrystals with highest half-wave potential (0.893 V), mass activity (0.127 A mg −1 ), and specific activity (0.926 mA cm −2 ) in ORR. Additionally, this alloy nanocrystals follow an efficient four-electron reduction pathway and exhibit excellent long-term stability over 10,000 cycles. Density functional theory calculations suggest that the outstanding ORR performance stems from the minimal downhill energy gradient in the rate-determining step, and the reduced oxygen adsorption energy on the PdNi alloy (311) crystal plane. This innovative strategy adds more potentialities for development and commercial application in fuel cells.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
高影响因子
ACS Sensors
·
2025
·
IF 9.1
Kang Yang,Bin Zhou,Hong Zhou,Tianrun Zheng,Yueying Liu,Xishuang Liang,Fengmin Liu,Geyu Lu
Rapid and robust ppb-level H2S sensing is of great importance for environmental monitoring, industrial safety, food quality control, and disease screening. However, improving the H2S sensing properties of semiconductor oxides under low-power conditions remains a significant challenge. In this work, an acid etching method was utilized to precisely control the elemental distribution in bimetallic nanoalloys. By tailoring the Ni distribution in PdNi alloy nanoparticles anchored on ZnO nanosheets, an ultralow detection limit of 5 ppb for H2S was achieved at a working temperature of 140 °C. More importantly, the sensor also demonstrated fast response and recovery kinetics, with its superior antipoisoning performance attributed to the oxidation of H2S into SO2 instead of sulfates or sulfites, as evidenced by in situ FTIR spectroscopy. Additionally, density functional theory calculations were performed to elucidate the synergistic effect of the PdNi alloy, revealing that Pd atoms act as electron donors while Ni atoms facilitate H2S adsorption. This study provides a viable strategy for optimizing noble metal-modified oxide-based gas sensors.
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Jiawei Chen,Jiadong Chen,Danni Yu,Ming Zhang,Han Zhu,Mingliang Du
Efficient bifunctional electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) must be developed to realize an inexpensive water-splitting system for large-scale applications. Herein, a novel PdNi carbon nanofiber (PdNi/CNF) catalyst was synthesized by facile electrospinning and carbonization processes. The size and homogeneity of the Pd−Ni alloy nanoparticles (NPs) could be effectively tuned by controlling the molar feed ratio of metal precursors .The morphology and structure of the PdNi/CNFs were characterized, and the working electrodes fabricated from the prepared catalyst mats were directly employed in the HER and OER. The PdNi/CNFs-1:2 catalyst exhibits high catalytic activity in the HER with a low overpotential of 55 mV at a current density of 10 mA cm −2 in an acidic solution. Moreover, under 1 M KOH electrolyte, an overpotential of 187 mV is required in the HER over the catalyst to arrive 10 mA cm −2 and an overpotential of 289 mV is achieved in the OER at the same current density. The superior HER and OER activities of the PdNi/CNFs are attributed to the synergistic effects of the PdNi alloy nanoparticles (NPs) assembled on the CNFs. This work provides a simple route for synthesizing highly efficient bifunctional electrocatalysts from 3d transition metals and a small amount of noble metals for hydrogen and oxygen evolution reactions.
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DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2026
·
IF 5.2
Wenqing Deng,Shun Xiao,Luna Ruan,Haojian Kang,Laixi Zou,Lihua Zhu
Herein, a series of PdNi alloy electrocatalysts supported on N, P-codoped carbon (denoted as PdNi/NPC) with controlled Pd:Ni mass ratios (Pd 1 Ni 2 /NPC, Pd 1 Ni 1 /NPC, and Pd 2 Ni 1 /NPC) were synthesized. Among them, Pd 1 Ni 1 /NPC demonstrated superior mass activity and stability for both the methanol and ethanol oxidation reactions. For the ethanol oxidation reaction (EOR) in 1.0 M KOH containing 1.0 M CH 3 CH 2 OH, the mass activity of Pd 1 Ni 1 /NPC reached 2.77 A mg Pd -1 , which is about 12-fold higher than that of commercial Pd/C. Moreover, after a 10,000 s chronoamperometry (CA) stability test, it retained a mass activity of 2.61 A mg Pd -1 . Under alkaline conditions (1.0 M KOH + 1.0 M CH 3 OH) for the methanol oxidation reaction (MOR), Pd 1 Ni 1 /NPC exhibits a mass activity of 1.24 A mg Pd -1 , surpassing that of commercial Pd/C by a factor of six. Following 10,000 s of stability testing, the catalyst maintained a mass activity of 1.17 A mg Pd -1 . These improvements are ascribed to the electronic interaction between Pd and Ni, involving electron transfer from Pd to Ni. This interaction weakens the adsorption of reaction intermediates (e.g., CO ad ), promotes CO desorption and oxidation, and thereby enhances the durability of PdNi/NPC. The optimal catalytic performance observed at a Pd:Ni mass ratio of 1:1 indicates that an appropriate stoichiometry is crucial for enhancing electrocatalytic activity.
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DOI
高影响因子
Scientific Reports
·
2026
·
IF 3.9
Zhang Zutao,Xiao Peiyuan,Mei Jinping,Zhang Xinyu,Dai Anni,Wang Lei,Yao Qiufang
Chlorinated pharmaceuticals like diclofenac (DCF) pose persistent environmental risks due to their bioaccumulation and toxicity, necessitating advanced remediation strategies. Herein, an integrated electrochemical system was developed, combining a self-nitrogen-doped carbon nitride (CN)-supported PdNi (CN@PdNi) cathode for electrocatalytic hydrodechlorination (ECH) with a CN anode for oxidative mineralization in a single, sequential process. The CN@PdNi cathode achieved 98.6% ECH efficiency, selectively cleaving C–Cl bonds to mitigate toxicity, which is attributed to its structural merits, including a well-dispersed, albeit partially clustered, nanoparticle distribution, metallic Pd/Ni phases, predominant Pd 0 /Ni 0 states, and enhanced porosity. Subsequent CN anodic oxidation enabled 96.8% total organic carbon (TOC) removal, ensuring near-complete mineralization. Mechanistic studies via Electron paramagnetic resonance (EPR), quenching, LSV, and Tafel slopes revealed atomic hydrogen (*H) generated at Pd 0 sites as the primary reactive species, augmented by electron transfer. The system exhibited robust performance across varied conditions and exceptional stability (< 1% efficiency loss over 11 consecutive cycles). Toxicity assessments showed 3–5 Log 10 unit reductions (ECOSAR) and mung bean germination rates improving from 68.7 to 99.8%. This dual-functional detoxification-mineralization strategy overcomes the limitations of single-step processes and offers a scalable, sustainable solution for efficient remediation of halogenated pollutants.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Ning Sui,Tao Wang,Qiang Bai,Ruiping Yue,Haoran Jiang,Hailian Xiao,Manhong Liu,Lina Wang,Zhiling Zhu,William W. Yu
We report a facile synthesis of ternary Au@PdNi core-shell nanoparticles (C-SNPs). Au NPs with 15 nm in diameter served as seeds, Pd 2+ and Ni 2+ were co-reduced on the surface of Au NPs to obtain C-SNPs. These C-SNPs exhibited outstanding catalytic performance (5891 mA mg Pd −1 ) and stability for ethanol oxidation reaction (EOR). The activity was 9.48 times higher than the commercial Pd/C (20% wt). The catalytic mechanism was investigated, and the enhanced catalytic performance of Au@PdNi C-SNPs was mainly attributed to electronic effects between Pd and Au/Ni, and the unique core-shell nanostructure . The present work provides a strategy for rational design of ternary metallic core-shell nanocatalysts, which can achieve high catalytic activity and durability.
研究领域:
材料科学
·
电化学
·
纳米技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）