Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 30
·11949-11956
·
IF 8.262
Lian-Kui Wu,Xin-Yu Liu,Ji-Ming Hu
Ti-supported IrO2 or RuO2 oxide coated electrodes are widely used for the oxygen evolution reaction (OER) in acidic media. Electrocatalytic activity and long-term stability need to be further improved for these types of electrodes. A highly porous and well-adhered electrodeposited SiO2 (e-SiO2) film is proposed as the interlayer in this work to meet the above-mentioned requirements. The results show that the active oxide fully fills in the porous network throughout the whole thickness of the e-SiO2 film, to form “total-depth” highly porous oxide electrocatalytic coatings. For this reason, more than 1 order of magnitude higher apparent activity towards the OER at the Ti/e-SiO2/IrO2 (or RuO2) electrode is achieved compared to that of the conventional Ti/IrO2 or Ti/RuO2 electrode. Literature survey indicates that these novel electrodes are one of the most active Ti electrodes ever reported. The service life of this type of electrode is also obviously enhanced due to the “inter-locking” structure formed between the active oxide layer and e-SiO2 film.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
Precision Chemistry
·
2024
·
IF 0
Xianbing Miao,Jingda Zhang,Zhenpeng Hu,Shiming Zhou
Elucidating the electronic factors dominating the adsorption properties of transition-metal oxides is essential to construct highly efficient oxygen-evolving catalysts for hydrogen production by water splitting but remains a great challenge. Electron correlation from on-site Coulomb repulsion (U) among d-electrons is generally believed to significantly affect the electronic structure of these materials; however, it has long been neglected in studying their adsorption properties. Here, by choosing ruthenium oxide as a model system, we demonstrate the role of electron correlation on the electrocatalytic activity toward oxygen evolution reaction (OER). Our density functional theory plus U calculations on rutile RuO2 reveal that the electron correlation can tune the adsorption energies for oxygenated intermediate and optimize them after the metallic oxide being a Mott insulator upon increasing U. By regulating the RuO6 octahedral network, we constructed and synthesized a series of strongly correlated ruthenium oxides, where the Mott insulating ones indeed exhibit a superior OER performance to the metallic RuO2. Our work builds a bridge between the electrochemistry and Mott physics for transition-metal oxides, opening a new avenue for designing advanced catalysts.
研究领域:
材料科学
·
物理化学
·
能源技术
✓ 已验证
DOI
Journal of Energy Chemistry
·
2025
·
IF 14.9
Xuyan Zhou,Zijie Yang,Yinnan Qian,Zhaoyan Luo,Lei Zhang,Qianling Zhang,Chuanxin He,Zhengtang Luo,Xiangzhong Ren
Oxygen evolution reaction (OER) is widely recognized as a bottleneck of water electrolysis. To determine the underlying reaction mechanisms, particularly the relative contribution of the adsorbate evolution mechanism (AEM) and lattice-oxygen participation mechanism (LOM), we conduct a comprehensive investigation combining Density Functional Theory (DFT) calculations and experimental validation. Our theoretical analysis of doped RuO 2 catalysts reveals that heteroatom doping (Ni, Cu, and Zn) induces significant local charge transfer, leading to the increased charge state of Ru and the downshifted d -band center. This, in turn, enables the mechanism switching from the conventional AEM to the more efficient LOM, and finally improves OER activity. We also establish a simple yet powerful descriptor, N e of Ru (representing charge density of Ru sites), which enables accurate prediction of both catalytic activity and stability. Guided by these theoretical predictions, we successfully synthesize a Ni-doped RuO 2 catalyst, which exhibits excellent OER activity and stability in acidic media, achieving an overpotential of just 156 mV and maintaining stability for 4000 h at 10 mA cm −2 , significantly surpassing the performance of the commercial RuO 2 . These findings not only provide fundamental insights into the mechanism-switching behavior in OER catalysis but also offer a practical strategy for designing high-performance, stable electrocatalysts for acidic water electrolysis.
研究领域:
电催化
·
材料化学
·
物理化学
·
能源科学
·
纳米材料
·
电化学水裂解
✓ 已验证
产品关联
DOI
高影响因子
SOLID STATE IONICS
·
2021
·
IF 3.785
Songzhao Wang,Jiwen Hu,Xuefeng Gui,Shudong Lin,Yuanyuan Tu
Ni 12 P 5 has excellent electrochemical properties due to the existence of a large number of Ni P bonds with abundant phosphorus vacancies. RuO 2 has good electrical conductivity and catalytic activity , and its OER activity is very significant. In this paper, RuO 2 nanoparticles were loaded onto the surfaces of Ni 12 P 5 particles, forming RuO 2 /Ni 12 P 5 /C composite electrode catalytic materials which were prepared and applied to Li O 2 cells. The electrochemical tests reveal that the specific capacity of the Li O 2 battery with a RuO 2 /Ni 12 P 5 /C electrode reaches 4296 mAh g −1 , the cycle life reaches 56 cycles, and the over-potential is effectively controlled at the current density of 200 mA g −1 . This improvement is attributable to the effective adsorption of phosphorus vacancies in Ni 12 P 5 and the excellent OER catalytic activity of RuO 2 . Therefore, this work significantly enhanced the electrochemical performance of the cell, thus laying the foundation for the development of Li O 2 batteries.
研究领域:
电化学
·
材料科学
·
能源存储
·
催化化学
·
纳米材料
✓ 已验证
DOI
高影响因子
Science China-Technological Sciences
·
2022
·Vol. 65
·期 10
·2317-2324
·
IF 3.903
Gao HongMei,Xiao MeiLing,Li GuoQiang,Gao LiQin,Meng QingLei,Luo ZhaoYan,Luo ErGui,Liu ChangPeng,Jin Zhao,Ge JunJie,Xing Wei
The material innovation is prerequisite to accelerating sluggish oxygen evolution reaction (OER) kinetics, thus promoting the realization of hydrogen energy community. Herein, we develop an oxygen-vacancy-rich TiO 2 supported RuO 2 catalyst (RuO 2 @r-TiO 2 ) towards improved OER activity and stability. The oxygen vacancy on TiO 2 not only supplies electrons to produce lower valence Ru, but also provides sufficient anchoring site for the deposition of RuO 2 nanocrystal. Beyond that, it can generate strong electronic interaction between TiO 2 and supported RuO 2 , and thereby tailors the intermediates’ adsorption energy on the RuO 2 surface. As a result, the derived RuO 2 @r-TiO 2 catalyst exhibits superior OER activity and stability with the overpotential of 211 mV at a current density of 10 mA cm −2 and negligible activity degradation after 6 h operation, outperforming the non-oxygen-vacancy counterpart (223.3 mV, 12.75% activity loss) and RuO 2 catalyst (234.6 mV, 42.86% activity loss).
研究领域:
材料科学
·
电化学
·
催化化学
·
能源材料
·
纳米科技
·
物理化学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2022
·Vol. 14
·期 24
·e202201010
·
IF 5.497
Yanping Hu,Jing Zhou,Xuzhuo Sun,Jing Chen,Bo Li,Yujia Wang,Ning Wang
Graphical Electrocatalytic water-splitting : A facile reduction-hydrolysis strategy was developed to fabricate a Ru−RuO 2 hybrid on various substrates (Ni foam, graphene and CNT) as bifunctional electrocatalysts for water-splitting. Engineering bifunctional nanocomposites with pronounced interfacial structure represents an effective design strategy for water-splitting catalysts. Herein, a facile reduction-hydrolysis method is described for the fabrication of Ru−RuO 2 hybrid nanocomposites on various substrates [Ni foam (NF), carbon nanotubes (CNT) and graphene oxide (GO)] as overall water-splitting catalysts. Polydopamine (PDA) is the key element for simultaneously fabricating the Ru−RuO 2 hybrids as a moderate reductant by controlling the reduction rate. In the synthesis process, a gradual reduction of Ru 3+ to Ru 0 in the presence of PDA occurred during the hydrolytic process of Ru 3+ to form RuO 2 ⋅ n (H 2 O). After calcination, Ru−RuO 2 hybrids with tight interfacial contacts and high electrical conductivity exhibited excellent performance for both HER and OER. Especially, Ru−RuO 2 hybrids on the NF (Ru−RuO 2 /NC/NF) achieved outstanding catalytic activity toward HER and OER with overpotential of 24 mV and 223 mV at a current density 10 mA cm −2 in alkaline solution, respectively. This work provides a new method for facile synthesis and engineering of Ru−RuO 2 nanoparticles on various substrates for boosting the HER/OER performance.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jia Hui,Meng Xiang,Jianxiang Chen,Shilong Zhou,Yin Cheng,Zhou Yang
Water splitting is the most feasible way of obtaining hydrogen energy, but the high overpotential of the electrocatalytic materials conventionally used for water splitting create a bottleneck in the process. Herein, we prepare a NiS x /C-780 electrocatalyst derived from lignin and nickel that exhibits good electrocatalytic properties and for which the overpotential of 358 mV at 10 mA cm -2 for the oxygen evolution reaction (OER) and the Tafel slope of 107.7 mV dec -1 are superior to those of commercial RuO 2 . This study serves as a reference for designing low-cost and environmentally friendly electrocatalysts for water splitting.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Yin Qin,Sihao Deng,Xiao-Ye Zhou,Bin Cao,Zhehan Ying,Zilin Yan,Zheng Zhong,Lunhua He,Kaikai Li,Tong-Yi Zhang
RuO2, the benchmark catalyst for the oxygen evolution reaction (OER), has traditionally been considered Pauli paramagnetic; however, recent findings have demonstrated its antiferromagnetic (AFM) properties, hinting at the opportunity to enhance RuO2’s OER performance by manipulating its magnetic traits. In this study, we successfully induced weak ferromagnetism in commercial RuO2, transitioning it from an AFM state using an electrochemical sodiation method. This process resulted in high activity, achieving an overpotential of 145 mV to reach 10 mA cm–2 and extending the service hours by more than 13 times compared to pristine RuO2 in 0.5 M H2SO4. A combination of experimental and theoretical analyses indicated that the sodiation triggers significant surface compressive stress, leading to lattice distortion and disruption of the pristine structural symmetry of RuO2. Consequently, orbital degeneration ensues, prompting individual spin-up d electrons to jump to the high-spin state. This mechanism drives the conversion from AFM to weak FM behavior for RuO2, ultimately yielding exceptional catalytic activity and stability.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
·
固态物理
·
表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chem
·
2023
·
IF 23.5
Na Yao,Hongnan Jia,Juan Zhu,Zhaoping Shi,Hengjiang Cong,Junjie Ge,Wei Luo
The development of highly efficient and stable electrocatalysts toward the acidic oxygen evolution reaction (OER) is essential for the practical application of proton-exchange membrane water electrolyzers. Although Ru oxides possess remarkable initial activity toward the acidic OER due to the kinetically favorable lattice oxygen oxidation mechanism pathway, the soluble high-valence oxygen-vacancy intermediate (∗Vo-RuO 4 2− ) may accelerate the dissolution of Ru species, leading to dramatically decreased activity and unsatisfied long-term stability. Here, we developed a robust metal-organic framework anchored strategy by stabilizing atomically isolated Ru oxide on UiO-67-bpydc with strong coordinating pyridine ligands. Theory calculations and experimental results including in situ Raman, X-ray absorption spectroscopy, and 18 O-labeled differential electrochemical mass spectrometry reveal that the Ru–N bonds between Ru oxide and UiO-67-bpydc could not only accelerate the participation of lattice oxygen during the OER process but also stabilize the soluble ∗Vo-RuO 4 2− intermediate, which contribute to the enhanced OER performance and long-term stability of up to 115 h.
研究领域:
电催化
·
材料化学
·
能源科学
·
无机化学
·
物理化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Jiaming Sun,E. Lei,Chunhui Ma,Zhenwei Wu,Zhou Xu,Yushan Liu,Wei Li,Shouxin Liu
We prepared carbon aerogel/RuO 2 composites with three-dimensional microtubes based on renewable natural kapok fibers by combining a NaClO 2 pretreatment, CO 2 activation and loading of RuO 2 nanoparticles . The electrochemical performance of the material was optimized by tuning the carbonization temperature. The composite calcined at 800 °C for 2 h and activated by CO 2 for 30 min possessed an integrated tubular structure and moderate pore size distribution . This composite material also showed highest specific capacitance of 433 F g −1 at a current density of 1 A g −1 with a capacitance retention of 91.5% for 2000 cycles in 3 M KOH solution in three-electrode system. The maximum energy density was 8.92 Wh kg −1 at 558.12 W kg −1 at a cell voltage of 1 V in 3.0 M KOH aqueous electrolyte in a symmetric device. We attribute the reversible capacity of the obtained bio-derived carbon aerogel/RuO 2 composites to the high-speed flow of the electrolyte in the unique hollow tubular structure, the appropriate pore size distribution and the synergetic effect of the high capacitance of RuO 2 and good stability of the carbon material.
研究领域:
材料科学
·
纳米科技
·
电化学
·
能源存储
·
功能材料
·
可持续材料
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yue Shi,Hongfu Miao,Jianyang Gao,Feifei Liu,Ying Deng,Hongdong Li,Jingqi Chi,Caixia Li,Fusheng Liu,Jianping Lai,Lei Wang
The sluggish kinetics and inherent instability over the Ru/RuO 2 clusters are still enormous challenges in proton exchange membrane (PEM) water electrolyzer. Herein, we innovatively report synergistic modulation of dynamic electron modification and strong metal-support interaction (SMSI) to activate and stabilize bifunctional fluorine doped Ru/RuO 2 clusters anchored on carbon nanotube (CNT), thus achieving efficient and stable acidic overall water splitting. Theoretical and experimental studies found that surface metal-fluorine modification layer could dynamically regulate the interfacial electronic environment to stabilize and activate multiple active Ru species; and the SMSI between Ru/RuO 2 cluster and CNT maintains stable electronic environment for dynamic electron modification and avoids migrating or shedding of active species in acidic environment. Therefore, the PEM electrolyzer assembled with optimal F 5.5 -Ru/RuO 2 @CNT can operate stably for 100 h at a high current density of 100 mA cm −2 , which is the first time that bifunctional Ru-based nanocatalysts applied to PEM device at a high current density.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Xudan Li,Hanwei He
Cobalt hydroxide nanosheets/ruthenium oxide (Co(OH) 2 /RuO 2 ) nanocomposite on nickel foam was successfully synthesized via a simple electrodeposition process as an advanced supercapacitor electrode material. The microscopy studies reveal that RuO 2 nanoparticles are loaded uniformly on interconnected Co(OH) 2 nanosheets forming a three-dimensional (3D) network. The performance optimization of composite is come true through adjusting deposition time of RuO 2 nanoparticles. The electrochemical tests indicate that the optimized Co(OH) 2 /RuO 2 nanocomposite displays excellent super-capacitive properties. The specific capacitance is up to 2168 F g −1 as the current density is 1 A g −1 . Compared with the pure Co(OH) 2 and RuO 2 , the capacitance of the Co(OH) 2 /RuO 2 composite increases by 57% and 80%, respectively. The capacitance maintains at 86.0% after 5000 charging and discharging loops at the constant current density of 5 A g −1 , while the pure Co(OH) 2 only maintains 71.7% of the original capacitance after 5000 loops. The asymmetric capacitor assembled using Co(OH) 2 /RuO 2 nanocomposite as positive electrode and activated carbon (AC) as negative electrode exhibits a high energy density of 58.4 W h kg −1 at a power density of 1.2 kW kg −1 . The good pseudocapacitance behavior of the Co(OH) 2 /RuO 2 composite is mainly in virtue of the good synergies between Co(OH) 2 and RuO 2 insuring large surface area, rich electrochemical reactive sites, the short diffusion pathways of ions and good electroconductivity during the charge-discharge process.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 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）