APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yinghao Guo,Aiqing Cao,Lin Zhang,Marshet Getaye Sendeku,Yaping Li,Yun Kuang,Fengmei Wang,Xiaoming Sun
The chlorine evolution reaction is an anodic reaction in the chlor-alkali process, which utilizes dimensionally stable anodes (DSA) with large amounts of noble metals like iridium. Cheaper chlorine evolution anodes with high selectivity and stability are highly appealing but challenging. Here, a polymetallic oxide consisting of Sn, Ru, Nb, and Ti elements is synthesized on Ti felt for catalyzing chlorine evolution reaction. In particular, the Ru 0.3 Sn 0.6 Nb 0.1 O 2 film on Ti felt (i.e., Ru 0.3 Sn 0.6 Nb 0.1 O 2 /Ti) demonstrates a low overpotential of 42 mV at 10 mA cm −2 in 5 M NaCl (pH= 2) along with high Cl 2 selectivity (96.0 %) and mass activity (54.2 A g Ru −1 ) at 1.41 V versus reversible hydrogen electrode, which is 16 times higher than that of DSA electrode (3.2 A g Ru+Ir −1 ). Significantly, this anode can stably work for > 500 h at a current density of 100 mA cm −2 without attenuation. The flow cell fabricated with the Ru 0.3 Sn 0.6 Nb 0.1 O 2 /Ti anode and Pt/C cathode possesses excellent stability with a Cl 2 selectivity of 93 %, surpassing the flow cell fabricated with the DSA anode (81 %). The Ru 0.3 Sn 0.6 Nb 0.1 O 2 /Ti electrode exhibits low noble metal costs (7 % of DSA), and lower energy cost (82.5 % of DSA), but similar durability, showing great potential for industrial application.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xing Yang,Yongqi Liu,Xiaohui Niu,Ke Chu
Metalloporphyrin ligands themselves can participate in the redox process, making them beneficial in promoting the multielectron catalytic process of the oxygen evolution reaction (OER). However, OER catalysts synthesized by traditional chemical strategies face challenges in water electrolysis. We synthesized high-performance and stable alkaline and acidic OER electrocatalysts loaded with ultrasmall iridium clusters by taking advantage of the attraction and confinement of Ir atoms by the Ir–N bonds formed by the porphyrin cavity. The N in the porphyrin cavity forms an Ir–N bond with Ir so that Ir carries a negative charge and attracts Ir atoms to form ultrasmall Ir clusters above the cavity to adjust the electronic structure of the Ir clusters. The resulting catalyst Tpyp-Ir(IrOX) exhibits a small overpotential (242 and 259 mV) at a current density of 10 mA cm–2 in alkaline and acidic conditions and demonstrates good long-term operational stability. In addition, Tpyp-Ir(IrOX) exhibits a higher transition frequency (TOF) (1.69 O2 s–1 at 300 mV) in 1 M KOH, which is 7 times that of Ir/C.
研究领域:
材料科学
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催化化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Dongze Li,Wei Tu,Yuxiang Jin,Chao Wang,Song Jin,Wei Liu,Erhong Song,Zhangquan Peng,Junyuan Xu,Ligang Feng
Understanding the intricate mechanisms from material fabrication to catalytic reaction is crucial in energy chemistry. Herein, we elucidate the underlying mechanisms from catalyst to catalysis on Ir-segregated SrIrO 3 (Ir/SrIrO 3 ) as an efficient hydrogen evolution reaction (HER) catalyst in acidic conditions. During the phosphorization-assisted reduction process, in-situ spectroscopic analysis revealed that hydrogen radicals (H·) from the dissociation of P-H bonds attack the lattice oxygen at edge Ir-O sites, resulting in the segregation of Ir atoms and the formation of robust Ir-O interfacial structures between exsolved Ir clusters and the oxygen sites in SrIrO 3 . These interfacial structures are essential for the high performance of HER, while SrIrO 3 provides structural stability. The protons in the electrolyte are activated at the Ir nanocluster sites, incorporating oxygen in SrIrO 3 through the Ir-O interface, forming a reconstructed Ir-OH structure. This structure maintains both thermodynamic and electrochemical stability by adjusting hydrogen diffusion, embedding, and surface hydrogen coverage to sustain dynamic equilibrium during the catalytic process. Theoretical analysis confirms the necessity of the stable Ir-O interface via Ir- 5d and O- 2p orbital hybridization and hydrogen intercalation, optimizing charge redistribution, hydrogen bond length, and hydrogen adsorption free energy for enhanced HER kinetics. This study provides new insights into catalyst development by elucidating the relationship between catalyst structure and catalytic performance.
研究领域:
能源化学
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催化材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Defu Yin,Zewei Hu,Mingya Liu,Jingyun Zhang,Hanli Zheng,Yunxi Hou,Shitao Yu,Lu Li,Shiwei Liu,Yue Liu
The highly stereoselective hydrogenation of α-pinene was very important and challenging in the utilization of natural products at mild conditions. Here, we reported a core–shell catalyst coated with Ir metal particles by mesoporous silica shell, and revealing the dependence of reducing agents during the preparation process. The prepared nano catalyst exhibited excellent performance in the hydrogenation of chiral substance α-pinene, especially under very mild conditions (40 °C, 1 MPa H 2 and 2 h), with a yield of cis -pinane reaching ∼99 %. The characterization methods revealed that the excellent performance was attributed to the strong hydrogenolysis ability of Ir particles. DFT results further indicated that α-pinene can stably adsorb on the edge sites of Ir metal in a cis structure, thereby achieving highly stereoselective hydrogenation. This work utilized heterogeneous catalysis to achieve performance close to that of homogeneous catalysts. The stable core shell structure greatly prolonged the lifespan of the catalyst and overcame the drawbacks of homogeneous catalysts. This work provided more reference cases for chiral hydrogenation.
研究领域:
催化
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材料科学
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化学工程
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有机化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
·
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
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Huiyu Sun,Shudi Yu,Jiongting Yin,Jie Li,Jun Yu,Tianpeng Liu,Wanyu Liang,Nannan Zhang,Yangping Zhang,Changqing Ye,Mengyun Hu,Yukou Du
Electrolysis of water to produce hydrogen is an efficient, clean, and environmentally friendly hydrogen production method with unlimited development prospects. However, its overall efficiency is hampered by the slow oxygen evolution reaction (OER) with complex electron transfer processes. Therefore, designing efficient and low-cost OER catalysts is the key to solving this problem. In this paper, Ir-doped Co2P/Fe2P (abbreviated as Ir-CoFeP/NF) was grown on nickel foam through the strategies of low amount noble-metal doping and mild phosphating. Phosphide derived from a floral metal–organic framework (MOF) exhibits regular three-dimensional (3D) morphology and large active area, avoiding the stacking of active sites. The addition of Ir can effectively adjust the electronic structure, change the position of the d-band center, and increase active sites, thus enhancing the catalytic activity. Hence, the optimized catalyst exhibits unexpected electrocatalytic OER activity with an ideal overpotential of 213 mV at 10 mA cm–2, as well as a low Tafel slope of 40.63 mV dec–1. Coupling with Pt/C for overall water splitting (OWS), the entire device only needs an ultralow cell voltage of 1.50 V to achieve a current density of 10 mA cm–2. Besides, the OWS can be maintained for more than 70 h. This study demonstrates the superiority of Ir-doped phosphide in accelerating water oxidation.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF POLYMER ANALYSIS AND CHARACTERIZATION
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2013
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IF 1.233
Shunping Wang,Xiaodeng Yang,Qingquan Bai,Tianduo Li
A number of tertiary amines and organotin catalysts for the phenyl isocyanate- 1,2-propylene glycol reaction were investigated by using in situ FT-IR. The reaction rate of each hydroxyl group, which is defined as the ratio between the rate constant of the secondary hydroxyl group and the rate constant of the primary hydroxyl group, is described with a second-order equation. The influence of different catalyst concentrations as well as the reaction temperature is discussed. It is observed that the selectivity depends on temperature but not on concentration, and stannous octoate is the most effective catalyst. The thermodynamic parameters were determined for the catalyzed reactions, primary and secondary hydroxyl groups being differentiated.
研究领域:
化学工程
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材料科学
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催化化学
✓ 已验证
DOI
高影响因子
Nano-Micro Letters
·
2026
·Vol. 18
·期 1
·227
·
IF 36.3
Li Na,Cheng Weiren,Liu Yuying,Liu Ruiqi,Feng Sihua,Wang Huijuan,Lv Liyang,Liu Chenglong,Ma Jin,Wang Chao,Yan Wensheng
Monodisperse and substitute Co were doped into edge-sharing [IrO 6 ] octahedra of Ca 2 IrO 4 model catalyst, which usually present the intrinsic and strong stability for acid oxygen evolution reaction (OER)
The optimized Janus Co–Ir local structure triggers spin balance effect with optimal e g 1 orbital and uneven t 2g orbital despite the large crystal field of Ir, which co-promote the OER activity with a relatively stable crystal structure.
Different from the slowly kinetics of adsorbates evolution mechanism on Ca 2 IrO 4 , superoxide path mechanism occurs on Co doped Ca 2 IrO 4 based on the assignment of *OO on dual active sites of Ir and Co.
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Benyong Yang,Wentao Mu,Benedict Tsz Woon Lo,Sijie Liu,Zhihang Chen,Liam John France,Xuehui Li
NOx and CO formation is, at present, a consequence arising from fuel production, but their emission need not be. In this study, a series of novel Ir-containing TiO2-nanobelt catalysts were designed and prepared for the simultaneous removal of NOx and CO. Activity data demonstrates that the TiO2(B) support promotes NO reduction compared to anatase. Furthermore, reaction efficiency (RE), a measure of NOx consumption vis-à-vis that of CO, reveals that catalysts containing anatase promote CO oxidation more so than their TiO2(B) counterparts. Increasing Ir concentration over the latter promotes low-temperature catalytic performance, an effect believed to be linked to the formation of Ir0–IrO2 composites. In situ DRIFTS experiments reveal the relevance of nitrite/nitrate formation and consumption at 250 °C, a mechanism insinuated by the RE value. However, at 300 °C, both TOF and RE increase, signifying the participation of a faster and more-selective reaction, which appears consistent with the isocyanate-mediated pathway.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Hongbo Yu,Weiqiang Tang,Kaijie Li,Shuangliang Zhao,Hongfeng Yin,Shenghu Zhou
IrM (M = Fe, Co, and Ni) alloy nanoparticles (NPs) were synthesized in a solution by employing butyllithium as a reduction agent and oleylamine as a stabilizing agent, and the alumina-supported IrM bimetallic nanoparticles were tested for selective hydrogenation of various substituted nitroaromatics. The relevant characterizations including X-ray diffraction, X-ray photoelectron spectra, transmission electron microscopy, and diffuse reflectance fourier transform infrared with CO probes confirm that IrM NPs are uniform alloys. The obtained IrM/Al2O3 catalysts show significantly enhanced catalytic activity as well as selectivity relative to individual monometallic Ir catalysts, indicating a unique catalytic property of bimetallic alloy nanostructures. Among these bimetallic catalysts, IrNi/Al2O3 illustrate the highest activity and selectivity for hydrogenation of various substituted nitroaromatics. Calculations by density functional theory suggest that bimetallic structures of IrNi facilitate the reactant adsorption and product desorption, resulting in enhanced catalytic performance.
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
PubMed
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Hui Li,Hehe Wei,Longtao Zhang,Zixiang Su,Xueqing Gong
Highly active and durable noble metal-based catalysts for electrochemical hydrogen evolution are crucial for clean and renewable energy production, however, low abundance and high price hinder their development at industrial scale. Herein, we synthesized carbon-supported ultrafine iridium nanoparticles (Ir NPs/C) catalyst via solvothermal method which achieved ultralow overpotentials of 13 and 57 mV at the current density of 10 and 100 mA cm −2 for hydrogen evolution reaction (HER) in acidic media, respectively. The prepared Ir NPs/C catalyst also exhibited ultrahigh mass activity of 44.5 A mg −1 at the overpotential of 40 mV and outstanding long-term stability in HER performance for 12 h, remarkably superior to state-of-the-art commercial Pt/C catalyst (3.3 A mg −1 , fast decay) and commercial Ir/C catalyst (1.2 A mg −1 ). Furthermore, it possessed activities toward oxygen evolution reaction (OER) and overall water splitting. This work demonstrates evenly dispersed fine Ir NPs/C catalyst can facilitate highly efficient HER and provides inspiration for rational design of advanced electrocatalysts.
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
BIOINORGANIC CHEMISTRY AND APPLICATIONS
·
2023
·
IF 3.8
Jingfang Song,Jian He,Lin Yang,Weiguo Wang,Qinqin Bai,Wei Feng,Ranhui Li
To inhibit the growth of bacteria, the DA-PPI nanozyme with enhanced peroxidase-like activity was synthesized. The DA-PPI nanozyme was obtained by depositing high-affinity element iridium (Ir) on the surface of Pd-Pt dendritic structures. The morphology and composition of DA-PPI nanozyme were characterized using SEM, TEM, and XPS. The kinetic results showed that the DA-PPI nanozyme possessed a higher peroxidase-like activity than that of Pd-Pt dendritic structures. The PL, ESR, and DFT were employed to explain the high peroxidase activity. As a proof of concept, the DA-PPI nanozyme could effectively inhibit E. coli (G−) and S. aureus (G+) due to its high peroxidase-like activity. The study provides a new idea for the design of high active nanozymes and their application in the field of antibacterial.
研究领域:
生物化学
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材料科学
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微生物学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）