Journal of the American Chemical Society
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2021
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IF 15.419
Qi Wang,Zhe Zhang,Chao Cai,Maoyu Wang,Zhi Liang Zhao,Menghao Li,Xiang Huang,Shaobo Han,Hua Zhou,Zhenxing Feng,Lei Li,Jun Li,Hu Xu,Joseph S. Francisco,Meng Gu
Single-atom catalysts (SACs) with 100% active sites have excellent prospects for application in the oxygen evolution reaction (OER). However, further enhancement of the catalytic activity for OER is quite challenging, particularly for the development of stable SACs with overpotentials <180 mV. Here, we report an iridium single atom on Ni2P catalyst (IrSA-Ni2P) with a record low overpotential of 149 mV at a current density of 10 mA·cm–2 in 1.0 M KOH. The IrSA-Ni2P catalyst delivers a current density up to ∼28-fold higher than that of the widely used IrO2 at 1.53 V vs RHE. Both the experimental results and computational simulations indicate that Ir single atoms preferentially occupy Ni sites on the top surface. The reconstructed Ir–O–P/Ni–O–P bonding environment plays a vital role for optimal adsorption and desorption of the OER intermediate species, which leads to marked enhancement of the OER activity. Additionally, the dynamic “top-down” evolution of the specific structure of the Ni@Ir particles is responsible for the robust single-atom structure and, thus, the stability property. This IrSA-Ni2P catalyst offers novel prospects for simplifying decoration strategies and further enhancing OER performance.
研究领域:
材料科学
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催化化学
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能源化学
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Ruoyu Wei,Mansheng Liao,Lidan Sun,Qingfeng Zhang,Hong Zhang,Lei Zhang,Zhongxin Song
Developing highly efficient and low-cost bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in water splitting poses significant challenges. In this study, a novel bifunctional electrocatalyst, Irn-CoMoPOx, was achieved via incorporating low-loading Ir single atoms and clusters with the high-valence Mo6+ modified CoPOx nanosheets. The Irn-CoMoPOx catalyst demonstrates remarkable low overpotentials of 222 mV and 36 mV for the OER and HER, respectively, in delivering a current density of 10 mA cm–2. When employed as both the anode and cathode catalyst in overall water splitting, the Irn-CoMoPOx∥Irn-CoMoPOx configuration exhibits a superior cell voltage of 1.53 V, outperforming the benchmark Pt/C∥IrO2 electrolytic cell (1.60 V) for achieving the current density of 10 mA cm–2. Benefiting from the high-valence of Mo species, the metal–support interaction of Irn-CoMoPOx was greatly strengthened, resulting in an order of magnitude increase in the mass activity of Ir for the HER. The high valence of non-noble metals plays a crucial role in tuning the local electronic configurations and optimizing the adsorption energies of the intermediates, which synergistically improves the overall performance of Ir in water splitting. The study provides valuable insights for future research in the utilization of Ir-based bifunctional catalysts for overall water electrocatalysis applications.
研究领域:
材料科学
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电化学
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催化反应
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PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2024
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IF 3.8
Zhou Yaojiang,Wei Wen,Lei Wenli,Li Fudong,Shu Jiaxi,Deng Zixuan,Hui Wenyu,Zhao Yuanmeng,Shan Changsheng
The development of novel catalyst with high catalytic activity is important for electrochemical non-enzymatic glucose sensing. Here, iridium single-atom/nickel oxide nanoparticle/N-doped graphene nanosheet (Ir 1 /NiO/NG) with the loading of 1.13 wt% Ir was successfully synthesized for constructing electrochemical non-enzymatic glucose sensor for the first time. The morphology and structure of Ir 1 /NiO/NG were characterized by XRD, SEM, TEM, HRTEM, and XPS, and the presence of Ir SAs was confirmed by AC-HAADF-STEM. The Ir 1 /NiO/NG shows 65 mV lower oxidation potential and 3.3 times higher response current than Ni(OH) 2 /NG. In addition, Ir 1 /NiO/NG exhibits high sensitivity (70.09 μA mM −1 cm −2 ), excellent selectivity, low detection limit (2.00 μM), and great stability (91.53% current remaining after 21 days) for electrochemical non-enzymatic glucose sensing. The outstanding catalytic and sensing performance of Ir 1 /NiO/NG is mainly attributed to synergistic effect of Ir SAs, NiO nanoparticles, and highly conductive NG, which modulate the electronic and geometric structure of Ir 1 /NiO/NG. This work shows the promising potential of SACs in electrochemical sensing.
研究领域:
材料科学
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电化学
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分析化学
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DOI
PubMed
高影响因子
Bioactive Materials
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2025
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IF 20.3
Danyan Wang,Hui Jin,Yetao Shen,Dandan Wang,Jingjing He,Jinmiao Qu,Xiaojun He,Zhengli Jiang
Methicillin-resistant Staphylococcus aureus (MRSA) remains a major pathogen in ventilator-associated pneumonia and wound infections. To address the limitations of traditional antibiotics, we developed a novel iridium-based single-atom catalyst (Ir/CN SAC) anchored on a nitrogen-doped carbon matrix. Engineered for ultra-low metal loading and maximal active site exposure, this catalyst integrates robust photothermal and catalytic functionalities. Under second near-infrared (NIR-II, 1270 nm) irradiation, the Ir/CN SAC efficiently converts light to heat and catalytically generates reactive oxygen species (ROS), achieving a potent photothermal-catalytic synergistic effect. This dual-action mechanism enabled rapid bacterial eradication in vitro and significantly accelerated wound healing and lung tissue repair in MRSA-infected in vivo models. Transcriptomic analyses revealed downregulation of pro-inflammatory pathways, shedding light on the immunomodulatory roles of the treatment. Notably, the Ir/CN SAC exhibited negligible toxicity and enhanced peroxidase-mimicking activity via thermal activation. Collectively, the Ir/CN SAC presents a promising strategy for treating MRSA infections in wounds and the lungs via a synergistic treatment model.
研究领域:
生物医学工程
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纳米医学
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感染病学
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PubMed
高影响因子
Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Fang Jinjie,Wang Haiyong,Dang Qian,Wang Hao,Wang Xingdong,Pei Jiajing,Xu Zhiyuan,Chen Chengjin,Zhu Wei,Li Hui,Yan Yushan,Zhuang Zhongbin
Hydroxide exchange membrane fuel cells (HEMFCs) have the advantages of using cost-effective materials, but hindered by the sluggish anodic hydrogen oxidation reaction (HOR) kinetics. Here, we report an atomically dispersed Ir on Mo 2 C nanoparticles supported on carbon (Ir SA -Mo 2 C/C) as highly active and stable HOR catalysts. The specific exchange current density of Ir SA -Mo 2 C/C is 4.1 mA cm −2 ECSA , which is 10 times that of Ir/C. Negligible decay is observed after 30,000-cycle accelerated stability test. Theoretical calculations suggest the high HOR activity is attributed to the unique Mo 2 C substrate, which makes the Ir sites with optimized H binding and also provides enhanced OH binding sites. By using a low loading (0.05 mg Ir cm −2 ) of Ir SA -Mo 2 C/C as anode, the fabricated HEMFC can deliver a high peak power density of 1.64 W cm −2 . This work illustrates that atomically dispersed precious metal on carbides may be a promising strategy for high performance HEMFCs.
研究领域:
材料科学
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能源化学
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Zhaoping Shi,Ziang Wang,Hongxiang Wu,Meiling Xiao,Changpeng Liu,Wei Xing
The development of high-performance oxygen evolution reaction catalysts with low iridium content is the key to the scale-up of proton exchange membrane water electrolyzer (PEMWE) for green hydrogen production. Single-site electrocatalysts with maximized atomic efficiency are held as promising candidates but still suffer from inadequate activity and stability in practical electrolyzer due to the low site density. Here, we proposed a NaNO 3 -assistant thermal decomposition strategy for the preparation of high-density Ir single sites on MnO 2 substrate (NaNO 3 -H-Ir-MnO 2 ). Direct spectroscopic evidence suggests the inclusion of NaNO 3 accelerates the transformation of Ir-Cl to Ir-O coordination, thus generating uniform dispersed high-density Ir single sites in the products. The optimized H-Ir-MnO 2 demonstrates not only high intrinsic activity in a three-electrode set-up but also boosted performance in scalable PEMWE, requiring a cell voltage of only 1.74 V to attain a high current density of 2 A cm ‒2 at a low Ir loading of 0.18 mg Ir cm ‒2 . This work offers a new insight for enhancing the industrial practicality of Ir-based single site catalysts.
研究领域:
材料科学
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电化学
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高影响因子
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
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2022
·Vol. 39
·期 4
·2200013
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IF 3.467
Xinyi Wei,Jinfeng Zhang,Chang Liu,Xiaopeng Han,Yida Deng,Wenbin Hu
The construction of binary metal Pd-based catalysts is an effective strategy to enhance the activity of methanol oxidation reaction. Herein, atomically dispersed Ir single atoms doped to cuboctahedral Pd nanoparticles (Ir-SAs/Pd) as efficient catalysts for alkaline methanol oxidation are prepared via a simple chemical reduction method. The synthetic Ir-SAs/Pd catalysts exhibit the outstanding mass activity of about 1717.3 mA mg Pd −1 compared with pure Pd and commercial Pd/C in electrooxidation for methanol. Meanwhile, the introduction of Ir single atoms enhances the CO tolerance of Pd nanoparticles to a large extent. On the basis of density functional theory results, the enhanced catalytic performance and CO tolerance rely on the effective improvement of the electron dominance near Fermi level and the negative shift of the d-band center for Pd as a result of the electron redistribution between Pd and Ir atoms. This article will provide new insight into the design of high-performance binary metal catalysts for methanol oxidation in alkaline media.
研究领域:
化学
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材料科学
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催化科学
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DOI
高影响因子
Nanoscale
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2025
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IF 5.1
Runxin Li,Yangyang Dong,Heng Xu,Yifei Yuan,Jie Xu
High-valent metal single atoms generally exhibit exceptional electrocatalytic activity because of their rapid electron-transfer kinetics. However, their synthesis remains a formidable challenge owing to intrinsic instability under typical preparation conditions. Herein, atomically dispersed Ir3+ single atoms were successfully stabilized on a NiS2 matrix via a substitutional replacement of Ni lattice sites by Ir, followed by coordination with adjacent S atoms. The resulting catalyst delivers outstanding oxygen evolution reaction (OER) performance, achieving a current density of 10 mA cm−2 at an overpotential of only 190 mV. Density-functional theory calculations reveal that the high oxidation state of Ir upshifts the Ni d-band center toward the Fermi level, thereby strengthening OOH* adsorption and accelerating the OER kinetics. This work not only provides a robust strategy for constructing high-valent single-atom catalysts but also highlights the pivotal role of sulfide supports in stabilizing high oxidation states for advanced electrocatalysis.
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高影响因子
Nature Communications
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2022
·Vol. 13
·期 1
·1-10
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IF 17.694
Zhang Zhirong,Feng Chen,Wang Dongdi,Zhou Shiming,Wang Ruyang,Hu Sunpei,Li Hongliang,Zuo Ming,Kong Yuan,Bao Jun,Zeng Jie
The homogeneity of single-atom catalysts is only to the first-order approximation when all isolated metal centers interact identically with the support. Since the realistic support with various topologies or defects offers diverse coordination environments, realizing real homogeneity requires precise control over the anchoring sites. In this work, we selectively anchor Ir single atoms onto the three-fold hollow sites (Ir 1 /T O –CoOOH) and oxygen vacancies (Ir 1 /V O –CoOOH) on defective CoOOH surface to investigate how the anchoring sites modulate catalytic performance. The oxygen evolution activities of Ir 1 /T O –CoOOH and Ir 1 /V O –CoOOH are improved relative to CoOOH through different mechanisms. For Ir 1 /T O –CoOOH, the strong electronic interaction between single-atom Ir and the support modifies the electronic structure of the active center for stronger electronic affinity to intermediates. For Ir 1 /V O –CoOOH, a hydrogen bonding is formed between the coordinated oxygen of single-atom Ir center and the oxygenated intermediates, which stabilizes the intermediates and lowers the energy barrier of the rate-determining step.
研究领域:
催化
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材料科学
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电化学
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高影响因子
Nature Communications
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2022
·Vol. 13
·期 1
·1-12
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IF 17.694
Zhu Yiming,Wang Jiaao,Koketsu Toshinari,Kroschel Matthias,Chen Jin-Ming,Hsu Su-Yang,Henkelman Graeme,Hu Zhiwei,Strasser Peter,Ma Jiwei
Designing active and stable electrocatalysts with economic efficiency for acidic oxygen evolution reaction is essential for developing proton exchange membrane water electrolyzers. Herein, we report on a cobalt oxide incorporated with iridium single atoms (Ir-Co 3 O 4 ), prepared by a mechanochemical approach. Operando X-ray absorption spectroscopy reveals that Ir atoms are partially oxidized to active Ir >4+ during the reaction, meanwhile Ir and Co atoms with their bridged electrophilic O ligands acting as active sites, are jointly responsible for the enhanced performance. Theoretical calculations further disclose the isolated Ir atoms can effectively boost the electronic conductivity and optimize the energy barrier. As a result, Ir-Co 3 O 4 exhibits significantly higher mass activity and turnover frequency than those of benchmark IrO 2 in acidic conditions. Moreover, the catalyst preparation can be easily scaled up to gram-level per batch. The present approach highlights the concept of constructing single noble metal atoms incorporated cost-effective metal oxides catalysts for practical applications.
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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能源存储与转化
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PubMed
高影响因子
危险品化学品经营许可证（带存储）