APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Hongjing Wang,Wenxin Wang,Hongjie Yu,Qiqi Mao,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Engineering the interface between two-dimensional materials and polymers is of great importance to improve their catalytic performance for oxygen reduction reaction (ORR). Hence, polyaniline (PANI)-functionalized porous Pd metallene (Pd@PANI metallene) is prepared via a two-step strategy. Due to the ultrathin porous nanosheets and interfacial structure, the Pd@PANI metallene possesses sufficient active sites and optimized electronic structure, which exhibits superior oxygen reduction performance in alkaline electrolyte. The mass and specific activities for Pd@PANI metallene are measured to 1.79 A mg Pd −1 and 2.96 mA cm −2 , which are 11.9 and 9.30 times those of Pt/C (0.15 A mg Pd −1 and 0.32 mA cm −2 ), respectively. Additionally, the ORR performance and morphology of Pd@PANI metallene can be maintained after long-term stability testing, making it an excellent ORR catalyst. This work provides an effective interface engineering strategy to construct efficient two-dimensional ORR electrocatalysts to improve the performance.
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
ACS Nano
·
2021
·
IF 15.881
Shaoda Huang,Shuanglong Lu,Shun Gong,Qiuju Zhang,Fang Duan,Han Zhu,Hongwei Gu,Weifu Dong,Mingliang Du
Engineering the morphology and electronic properties simultaneously of emerging metallene materials is an effective strategy for enhancing their performance as oxygen reduction reaction (ORR) electrocatalysts. Herein, a highly efficient and stable ORR electrocatalyst, Fe-doped ultrathin porous Pd metallene (Fe–Pd UPM) composed of a few layers of 2D atomic metallene layers, was synthesized using a simple one pot wet-chemical method and characterized. Fe–Pd UPM was measured to have enhanced ORR activity compared to undoped Pd metallene. Fe–Pd UPM exhibits a mass activity of 0.736 A mgPd–1 with a loss of mass activity of only 5.1% after 10 000 cycles at 0.9 V versus the reversible hydrogen electrode (vs RHE) in 0.1 M KOH solution. Density functional theory (DFT) calculations reveal that the stable Fe dopant in the inner atomic layers of Fe–Pd UPM delivers a much smaller overpotential during O* hydrogenation into OH*. The morphology, porous structure, and Fe doping were verified to have enhanced ORR activity. We believe that the rational design of metallene materials with porous structures and interlayer doping is promising for the development of efficient and stable electrocatalysts.
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
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Qiqi Mao,Wenxin Wang,Yueji Wu,Ruidong Yang,Kai Deng,Hongjie Yu,Ziqiang Wang,Liang Wang,Hongjing Wang
Electrocatalytic alkynol semi-hydrogenation for the high-value chemicals alkenol with mild conditions and carbon-free emission is a potentially green and sustainable alternative to conventional thermocatalytic routes, which generally involves the design of electrocatalysts with high activity and high selectivity. Here, the rare-earth single-atom (Ln = La, Nd, Pr) coordinated Pd metallene (Ln 1 Pdene) is reported for electrocatalytic 2-methyl-3-butyn-2-ol (MBY) semi-hydrogenation reaction (MBY ESHR) to synthesis of 2-methyl-3-buten-2-ol (MBE). Typically, in alkaline medium containing 0.1 m MBY, MBY conversion and MBE selectivity of La 1 Pdene are as high as ≈97% and ≈95%, respectively, with excellent electrocatalytic stability. Meanwhile, in situ infrared spectra reveal the conversion of MBY to MBE during the dynamic electrocatalytic process. Theoretical calculations reveal that the interaction between La single-atom and Pd host triggers an unconventional transformation of the intermediate MBE* adsorption configuration during electrocatalytic hydrogenation, achieving the optimal desorption energy between La 1 Pd and target product and optimizing the reaction energy barriers to inhibit the over-hydrogenation of MBE. Moreover, La single-atom as the adsorption active site of the hydrogen supplier H 2 O effectively reduces the competition adsorption between the reactants MBY and H 2 O, rendering La single-atom and Pd host as the synergistic co-catalytic active sites to promote the electrocatalytic MBY semi-hydrogenation reaction.
研究领域:
材料科学
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电化学
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催化化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 19
·10222-10227
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IF 11.9
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Water electrolysis for hydrogen production consumes abundant electronic energy owing to the sluggish oxygen evolution reaction (OER), so the integration of the hydrogen evolution reaction (HER) with thermodynamically more favorable oxidation reactions is a promising strategy for energy-efficient hydrogen production. Herein, we propose the epitaxial confinement of rhodium nanoparticles (NPs) to palladium metallene (Rh/Pd metallene) for hydrogen production assisted by the hydrazine oxidation reaction (HzOR). The two-dimensional structure of Rh/Pd metallene provides sufficient active sites as well as a rapid charge transfer rate. The interface of Pd metallene with Rh NPs ensembles to modulate the electronic state, thus optimizing the adsorption energy of reaction intermediates. The Rh/Pd metallene exhibits splendid HER and HzOR activities, with overpotentials of 59 and 7 mV at 10 mA cm−2, respectively. In the two-electrode construction of a hydrazine oxidation-assisted water splitting system, the Rh/Pd metallene only needs a low overpotential of 0.19 V to produce hydrogen at a current density of 100 mA cm−2. This research offers a viable approach for designing nanosheet/nanoparticle heterojunction as an attractive modular platform for energy-saving hydrogen production.
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
ACS Nano
·
2024
·
IF 15.8
P Prabhu,Viet-Hung Do,Takefumi Yoshida,Yingtang Zhou,Hiroko Ariga-Miwa,Takuma Kaneko,Tomoya Uruga,Yasuhiro Iwasawa,Jong-Min Lee
Highly efficient, cost-effective, and durable electrocatalysts, capable of accelerating sluggish reaction kinetics and attaining high performance, are essential for developing sustainable energy technologies but remain a great challenge. Here, we leverage a facile heterostructure design strategy to construct atomically thin Os@Pd metallenes, with atomic-scale Os nanoclusters of varying geometries confined on the surface layer of the Pd lattice, which exhibit excellent bifunctional properties for catalyzing both hydrogen evolution (HER) and oxygen reduction reactions (ORR). Importantly, Os5%@Pd metallenes manifest a low η10 overpotential of only 11 mV in 1.0 M KOH electrolyte (HER) as well as a highly positive E1/2 potential of 0.92 V in 0.1 M KOH (ORR), along with superior mass activities and electrochemical durability. Theoretical investigations reveal that the strong electron redistribution between Os and Pd elements renders a precise fine-tuning of respective d-band centers, thereby guiding adsorption of hydrogen and oxygen intermediates with an appropriate binding energy for the optimal HER and ORR.
研究领域:
材料科学
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电催化
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能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Ziqiang Wang,Shan Xu,Qiqi Mao,Kai Deng,You Xu,Hongjing Wang,Hongjie Yu,Liang Wang
Designing two-dimensional (2D) materials functionalized with organic molecules is an effective tactic to enhance catalytic performances for the oxygen reduction reaction (ORR). Herein, we synthesize Pd metallene with in situ modification of polyethylenimine-ethylenediamine (Pd@PEI-EDA metallene), in which PEI-EDA serves as both the structure-directing agent and modifier. Pd@PEI-EDA metallene has ample active sites and tuneable electronic structures due to ultrathin nanosheets with abundant wrinkles and interfacial structure. In contrast with commercial Pd/C and Pt/C, Pd@PEI-EDA metallene displays preferable catalytic ORR performance under alkaline conditions. This work offers an in situ interface engineering tactic for the preparation of 2D polymer-metal electrocatalysts to boost the ORR performance.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Hongjing Wang,Xu Mu,Qiqi Mao,Kai Deng,Hongjie Yu,You Xu,Ziqiang Wang,Liang Wang
It is of great significance to develop electrocatalysts with high activity, selectivity, and stability for the electrosynthesis of H2O2. Here, we successfully prepare low-crystalline two-dimensional Pd metallene sulfide with isolated Pd sites and rich sulfur vacancies (L-PdS-Vs metallene) via a solvothermal method. The ultrathin two-dimensional structure, amorphous/crystalline heterophase structure, and plentiful sulfur vacancy of L-PdS-Vs metallene can provide sufficient active sites and a strong electronic effect. Moreover, sulfidation induces the isolation of Pd sites that can inhibit the dissociation of O–O bonds. As such, L-PdS-Vs metallene exhibits excellent electrocatalytic performance with high H2O2 selectivity (>90%) under a wide application potential. The average H2O2 productivity at 0.3 V is as high as 1.12 mol gcat–1 h–1, and the corresponding FE is over 90%. The sulfidation strategy has multiple advantages and provides an effective strategy for the design of high-performance 2e– ORR electrocatalysts.
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 FOOD COMPOSITION AND ANALYSIS
·
2025
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IF 4.6
Binbin Zhou,Xiaoqi Zheng,Yuan Li,Xuan Yang,Xinyi Li,An Liu,Liang Chen
Zearalenone (ZLE) is a fungal toxin, and ingestion of ZLE–contaminated food can lead to human cytogenetic toxicity, immunotoxicity and hepatorenal toxicity. This study developed an electrochemical sensor for detection of ZLE using palladium-metallene (Pd-Me) and polypyrrole molecularly imprinted nanotubes (PMIN). Pd-Me is a novel metal material with excellent conductivity, unique three-dimensional structure, numerous active sites, and high stability, which has attracted widespread interest in the field of electrocatalysis. However, there are few reports on its application in electrochemical sensors. The three-dimensional configuration prepared effectively avoids the problem of electrical conductivity attenuation caused by material stacking, thereby significantly improving the sensor sensitivity. The further introduced PMIN constructed three-dimensional imprinting chambers rich in specific recognition sites on the electrode surface, which can achieve precise capture and enrichment of ZLE molecules. Through condition optimization, the sensor achieves a linear range of 5 −1000 ng mL −1 with the detection limit of 1.55 ng mL −1 , and demonstrates good repeatability, stability and reproducibility (RSD = 2.16 %) in agricultural product analysis. Compared with the existing ZLE detection technology, this method has the advantages of simple operation, low cost, high sensitivity and good selectivity.
研究领域:
分析化学
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食品安全检测
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电化学传感
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分子印迹技术
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真菌毒素分析
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产品关联
DOI
高影响因子
Nature Communications
·
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Changjin Zhou,Jiahao Zhang,Hongyi Li,Dong Shao,Junlun Zhu,Wei Wen,Xiuhua Zhang,Zhengfang Tian,Shengfu Wang
As a key technology enabling green and sustainable chemical processes, nanozymes have significantly enhanced their catalytic efficiency and economic viability. Therefore, the development of a higher catalytic activity enzyme mimic to construct a portable and easily sensing strategy for sensitive, rapid, and convenient determination of a specific target is exceedingly elemental for an advanced sensing platform. Herein, we designed and prepared copper-doped palladium metallene (Cu–Pd metallene) with multiple enzyme-like activities for a sensitive colorimetric assay. The relevant kinetic parameters of Cu–Pd metallene with three kinds of enzyme-like activities were evaluated. The Michaelis–Menten constant of laccase mimic and oxidase mimic were calculated to be 0.041 and 0.51 mM, which exhibited high affinity to 2,4-dichlorophenol and 3,3′,5,5′-tetramethylbenzidine in the corresponding system, respectively. Inspired by its high catalytic activity, a simple and portable colorimetric sensing platform based on Cu–Pd metallene was developed to detect and distinguish epinephrine, phenolics, and thiram by UV–vis absorption spectrum and smartphone. Among them, the proposed method can detect epinephrine concentration in the range of 1–15 μg mL–1 by laccase-like activity, and a calculated reliable limit of detection is 0.18 μg mL–1. Owing to the inhibitory effect, the colorimetric sensing platform was used to analyze thiram, which presented a concentration range of 10–500 ng mL–1 and an acceptable detection limit of 4.4 ng mL–1. Considering the advantages of accuracy and ease of use of Cu–Pd metallene-based colorimetric sensing platform, it has great potential for real-time monitoring of relevant targets in poor areas.
研究领域:
纳米技术
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分析化学
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生物传感器
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酶模拟
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环境监测
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食品安全
·
即时检测
✓ 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）