Nature Communications
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2025
·Vol. 16
·期 1
·1-11
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IF 15.7
Wang Dawei,Lin Fangxu,Luo Heng,Zhou Jinhui,Zhang Wenshu,Li Lu,Wei Yi,Zhang Qinghua,Gu Lin,Wang Yanfei,Luo Mingchuan,Lv Fan,Guo Shaojun
Using metal oxides to disperse iridium (Ir) in the anode layer proves effective for lowering Ir loading in proton exchange membrane water electrolyzers (PEMWE). However, the reported low-Ir-based catalysts still suffer from unsatisfying electrolytic efficiency and durability under practical industrial working conditions, mainly due to insufficient catalytic activity and mass transport in the catalyst layer. Herein we report a class of porous heterogeneous nanosheet catalyst with abundant Ir-O-Mn bonds, achieving a notable mass activity of 4 A mg Ir −1 for oxygen evolution reaction at an overpotential of 300 mV, which is 150.6 times higher than that of commercial IrO 2 . Ir-O-Mn bonds are unraveled to serve as efficient charge-transfer channels between in-situ electrochemically-formed IrO x clusters and MnO x matrix, fostering the generation and stabilization of highly active Ir 3+ species. Notably, Ir/MnO x -based PEMWE demonstrates comparable performance under 10-fold lower Ir loading (0.2 mg Ir cm −2 ), taking a low cell voltage of 1.63 V to deliver 1 A cm −2 for over 300 h, which positions it among the elite of low Ir-based PEMWEs.
研究领域:
材料科学
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能源技术
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Yuhua Xie,Yumei Feng,Shuyuan Pan,Haifeng Bao,Yingjie Yu,Fang Luo,Zehui Yang
The commercialization of water-splitting technology strongly relies on the stable and high-performance electrocatalyst for hydrogen and oxygen evolution reactions (HER-OER). In this work, the nickel dopants in IrRu alloyed electrocatalyst for acidic water splitting activity are investigated. The incorporation of nickel dopants induces more oxygen atoms coordinating with Ir/Ru facilitating the formation of *OOH species via nucleophilic attack by H 2 O. Additionally, a fast surface reconstruction is achieved due to the electrochemical dissolution of Ni dopants; as a result, more oxygen species are incorporated, evidenced by in situ Raman spectroscopy and electrochemical impedance spectroscopy. Therefore, the mass activity for Ni@IrRu is enhanced by threefold than commercial IrO 2 in acidic OER catalysis. Moreover, the nickel dopants balance the hydrogen binding strength; as a result, only 609 mV overpotential is demanded to reach 1 A cm −2 in acidic HER catalysis. The polymer electrolyte membrane water electrolyzer (PEMWE) test indicates only 1.87 V is required to attain 2 A cm −2 , 160 mV lower than Pt/C-IrO 2 revealing its potential application in PEMWE.
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
Nature Communications
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2025
·Vol. 16
·期 1
·1-9
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IF 15.7
Zheng Wen-Xing,Cheng Xuan-Xuan,Chen Ping-Ping,Wang Lin-Lin,Duan Ying,Feng Guo-Jin,Wang Xiao-Ran,Li Jing-Jing,Zhang Chao,Yu Zi-You,Lu Tong-Bu
Ruthenium dioxide has attracted extensive attention as a promising catalyst for oxygen evolution reaction in acid. However, the over-oxidation of RuO 2 into soluble H 2 RuO 5 species results in a poor durability, which hinders the practical application of RuO 2 in proton exchange membrane water electrolysis. Here, we report a confinement strategy by enriching a high local concentration of in-situ formed H 2 RuO 5 species, which can effectively suppress the RuO 2 degradation by shifting the redox equilibrium away from the RuO 2 over-oxidation, greatly boosting its durability during acidic oxygen evolution. Therefore, the confined RuO 2 catalyst can continuously operate at 10 mA cm –2 for over 400 h with negligible attenuation, and has a 14.8 times higher stability number than the unconfined RuO 2 catalyst. An electrolyzer cell using the confined RuO 2 catalyst as anode displays a notable durability of 300 h at 500 mA cm –2 and at 60 °C. This work demonstrates a promising design strategy for durable oxygen evolution reaction catalysts in acid via confinement engineering.
研究领域:
材料科学
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电化学
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PubMed
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
Advanced Energy Materials
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2025
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IF 26
Heng Zhang,Lili Liu,Liu Pei,Dongdong Wang,Xindong Wang
The application of ruthenium-based catalysts in proton-exchange membrane water electrolyzers is impeded by lattice oxygen mechanism and the subsequent structural collapse. Herein, a design strategy for the preparation of N-doped RuO₂ using TiN nanoparticles as the nitrogen source is presented. The in- situ characterization and theoretical calculation reveal the optimized oxygen evolution reaction (OER) mechanism on the resulting N-RuO 2 /TiN catalyst. The incorporation of low-electronegativity N and the formation of interfacial Ru−O−Ti bridge structure lead to the redistribution of electron density on adjacent Ru sites, weakening the Ru–O covalency and inhibiting the reactivity of lattice oxygen during electrocatalytic OER. Meanwhile, the altered electronic structures also optimize the adsorption energy of intermediates, consequently facilitating the formation of the pivotal intermediate *OOH and enhancing the electrocatalytic activity. The N-RuO 2 /TiN electrocatalyst displays a extremely low OER overpotential of 159 mV at 10 mA cm −2 in 0.5 m H 2 SO 4 . Particularly, the water electrolysis single cell with N-RuO 2 /TiN as anode electrocatalyst conveys an extremely low voltage of 1.78 V at 3A cm −2 and degradation rate of 26 µV h −1 during a 1100 h operation at 1 A cm −2 . This work also provides an excellent catalyst for industrial-level electrolysis.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jiahao Yang,Zhaoping Shi,Yibo Wang,Hongxiang Wu,Jing Ni,Pengbo Wang,Meiling Xiao,Changpeng Liu,Wei Xing
Despite proton exchange membrane water electrolysis (PEMWE) being a commercially viable method for high-purity hydrogen production, the development of active and robust anode electrocatalysts with reduced iridium loading under high current density conditions remains highly challenging. Here, we report a core-shell nanostructured catalyst with a metallic titanium core uniformly covered by Ir nanoparticles (Ti@Ir). The spontaneously formed TiO x layer can effectively disperse Ir nanoparticles via interfacial Ti-O-Ir bonds, which in turn increases the oxidation state of Ir towards activated lattice oxygen reactivity, as confirmed by in-situ differential electrochemical mass spectrometry (DEMS). As a result, the Ti@Ir exhibits an overpotential of only 272 mV to reach 10 mA cm −2 , 17 mV lower than non-supported Ir nanoparticles, and a 3.82-fold higher mass activity at 1.53 V. Moreover, the Ti@Ir catalyst demonstrates strong stability during a 100-hour test at 10 mA cm −2 . Detailed analysis reveals that the oxidation of iridium close to the titanium core is suppressed. The huge potential for practical application is further confirmed in a PEMWE prototype, with a low iridium loading of 0.5 mg Ir cm −2 , significantly lower than the typical 2 ∼ 4 mg Ir cm −2 required for traditional catalysts. This Ti@Ir catalyst achieves a cell voltage of 1.858 V at an industrial-level current density of 2 A cm −2 and maintains stable operation for 1800 h with an exceptionally low voltage degradation rate of only 1.252 μV h −1 .
研究领域:
材料科学
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能源技术
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电化学
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DOI
高影响因子
ACS Nano
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2025
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IF 16
Susu Zhao,Qian Dang,Aiqing Cao,Marshet Getaye Sendeku,Hai Liu,Jian Peng,Yameng Fan,Hui Li,Fengmei Wang,Yun Kuang,Xiaoming Sun
Ruthenium (Ru)-based catalysts have demonstrated promising utilization potentiality to replace the much expensive iridium (Ir)-based ones for proton exchange membrane water electrolysis (PEMWE) due to their high electrochemical activity and low cost. However, the susceptibility of RuO2-based materials to easily be oxidized to high-valent and soluble Ru species during the oxygen evolution reaction (OER) in acid media hinders the practical application, especially under current density above 500 mA cm–2. Here, a manganese-doped RuO2 catalyst with the hydroxylated metal sites (i.e., H–Mn0.1Ru0.9O2) is synthesized for acidic OER assisted by hydrogen peroxide, where the hydroxylation results in the valence state of the Ru sites below +4. The H–Mn0.1Ru0.9O2 catalyst demonstrates an overpotential of 169 mV at 10 mA cm–2 and promising stability for an OER over 1000 h in an acidic electrolyte. A PEMWE device fabricated with the H–Mn0.1Ru0.9O2 catalyst as the anode shows a current density of 1 A cm–2 at ∼1.65 V, along with a low degradation over continuous tens of hours. Differential electrochemical mass spectrometry (DEMS) results and theoretical calculations confirm that H–Mn0.1Ru0.9O2 performs the OER through the adsorbate evolution mechanism (AEM) pathway, where the synergistic effect of hydroxylation and Mn doping in RuO2 can effectively enhance the stability of Ru sites and lattice oxygen atoms.
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
Molecular Catalysis
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2024
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IF 3.9
Ning Wang,Kai Zhang,Xiaohang Du,Hongtao Bai,Pan Xu,Jingde Li
Low-cost and high-performance catalysts towards hydrogen evolution reaction (HER) are essential in proton exchange membrane water electrolysers (PEMWE). Herein, an efficient and durable titanium dioxide supported low platinum-loading (TiO 2 -Pt) catalyst was fabricated. The prepared TiO 2 -Pt catalyst achieve an HER overpotential of 22 mV at 10 mA cm −2 and excellent durability performance in 0.5 M H 2 SO 4 . Electron transfer from TiO 2 to Pt species and the presence of large amounts of proton on TiO 2 -Pt surface are verified, which facilitates the Heyrovsky step and promotes the HER activity of TiO 2 -Pt. The PEMWE with TiO 2 -Pt membrane electrode assemblies requires 1.65 V cell voltage to reach 1 A cm −2 and kept stable in 300 h continuous test. The electricity cost for hydrogen production by TiO 2 -Pt catalyst is below the US DOE requirements by 2026. This work provides a promising strategy for the synthesis of high-performance low Pt-loading HER catalysts for low-cost hydrogen production.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Cheng Yan,Xiyu He,Yunzhu Du,Jing Li,Yongjian Su,Jiewei Yin,Qiaodan Hu,Fan Yang,Junliang Zhang
Reducing iridium loading in oxygen evolution reaction (OER) is a promising solution to promote the widespread deployment of proton exchange membrane water electrolyzers (PEMWEs). In this work, we synthesized SrTi 1- x Ir x O 3 ( x = 0, 0.25, 0.50, 0.75, 0.80 and 1) perovskites by the conventional sol-gel reaction route and evaluated their OER electrocatalytic activity and durability in 0.5 M H 2 SO 4 to reveal the critical role of B-site cations. The optimum composition, SrTi 0.25 Ir 0.75 O 3 , exhibited excellent activity with an overpotential of 294 mV to drive 10 mA cm −2 and marvelous durability with a negligible increase in the overpotential of 15 mV in 580 h, and even a remarkable durability with a small increase in the overpotential of only 30 mV after 140 h when performed at 100 mA cm −2 . Multiple characterizations combined with DFT calculations indicated that the bimetallic synergistic effect caused by mixture of Ti and Ir on the B-site decreased the band gap to improve electrical conductivity and induced electronic coupling between Ir and Ti to lower the energy barriers for OER. When assembled in the membrane electrode assembly (MEA), the optimum composition also showed a superb performance and excellent durability. Results of this work provide a new perspective for designing electrocatalyst with low iridium content for OER in PEMWEs.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
Small Structures
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2024
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IF 13.9
Xiaotong Wu,Chao Lin,Weibo Hu,Chao Fu,Lei Tan,Haifeng Wang,Faiza Meharban,Xiangxiang Pan,Pan Fu,Han-Don Um,Qi Xiao,Xiaopeng Li,Miho Yamauchi,Wei Luo
Proton exchange membrane water electrolysis (PEMWE) with high-purity H 2 and O 2 products and swift response to electricity fluctuation is of great interest for renewable energy, chemical and pharmaceutical industries. Ruthenium oxide shows promise as an alternative to iridium oxide catalysts in PEMWE but suffers from severe anodic corrosion. Herein, a pluralistic electronic structure modulation approach is presented to address the instability issue of Ru, by in situ growing Mn x Ru 1− x O 2 solid solution on MnO 2 , coated carbon fibers (Mn x Ru 1− x O 2 /MnO 2 /CFs). Due to higher ion electronegativity, Mn dopants in the Mn x Ru 1− x O 2 solid solution accept electrons, activating the Ru site. Simultaneously, the MnO 2 support donates electrons to prevent Ru site overoxidation and dissolution due to its lower work function than the Mn x Ru 1− x O 2 solid solution. As a result, the Mn x Ru 1− x O 2 /MnO 2 /CFs catalyst exhibits a low overpotential of 161 mV at 10 mA cm −2 and a remarkable stability exceeding 600 h. Profiting by its improved oxygen evolution reaction (OER) kinetic activity, the Mn x Ru 1− x O 2 /MnO 2 /CF-based PEMWE shows a low cell voltage of 1.9 V at 2 A cm −2 , and stably operate at current density of 500 mA cm −2 for 24 h. This work shows the potential of the pluralistic electronic structure modulation to boost activity and stability of Ru-based acidic OER electrocatalysts.
研究领域:
材料科学
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电化学
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可再生能源
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DOI
高影响因子
Molecular Catalysis
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2024
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IF 3.9
Xiaoting Zhang,Yu Qiu,Xiaohui Guo,Jing Chang,Yantu Zhang,Jiangbo Cao,Yiwei Jiang,Jiale Bai,Wei Wang,Jianan Tian,Xueli Li
The exploitation of highly active, cheap cost and durable electrocatalyst for acidic water oxidation reaction still presents a major technological and scientific challenge in proton exchange membrane water electrolysers (PEMWEs). Herein, a hybrid aerogel of oxygen defect-rich RuO 2 nanoparticles coupling with carbon (V O -RuO 2 @CA) was designed to promote their activity and stability during acid water oxidation. The optimized V O -RuO 2 @CA achieves an ultralow overpotential of 207 mV at 10 mA cm −2 for acidic water oxidation and sustains a prominent long-term stability during the 30 h chronopotentiometry test in 0.5 M H 2 SO 4 . Furthermore, V O -RuO 2 @CA exhibits high mass activities of 186.5 mA mg Ru −1 and TOF values of up to 2.07 s − 1 at an overpotential of 300 mV, being 17.7 and 4.8 times higher than commercial RuO 2 , respectively. Theory calculations and experimental results verify that the oxygen vacancies (V O ) could significantly weaken the binding energy of O* with respect to OOH* for the interfacial Ru centers between RuO 2 and carbon, rendering the increase of the intrinsic water oxidation activity and resistance to over-oxidation for RuO 2 . This research provides a novel pathway to explore remarkably efficient 3D porous hybrid aerogel electrocatalysts toward anodic electrocatalysts applications in PEMWEs.
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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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Yuan Bichen,Dang Qian,Liu Hai,Sendeku Marshet Getaye,Peng Jian,Fan Yameng,Cai Liang,Cao Aiqing,Chen Shiyao,Li Hui,Kuang Yun,Wang Fengmei,Sun Xiaoming
Low-cost ruthenium-based catalysts with high activity have emerged as promising alternatives to iridium-based counterparts for acidic oxygen evolution reaction (OER) in proton exchange membrane water electrolyzers (PEMWE), but the poor stability under high current density remains as a key challenge. Here, we utilize the synergistic complementary strategy of introducing earth-abundant Mn and Nb dopants in ruthenium dioxide (RuO 2 ) for Nb 0.1 Mn 0.1 Ru 0.8 O 2 nanoparticle electrocatalyst that exhibits a low overpotential of 209 mV at 10 mA cm −2 and good stability of > 400 h at 0.2 A cm − 2 in 0.5 M H 2 SO 4. Significantly, a PEMWE device fabricated with Nb 0.1 Mn 0.1 Ru 0.8 O 2 anode can operate continuously at least for 1000 h at 0.5 A cm −2 with 59 μV h −1 decay rate. Operando Raman spectroscopy analysis, differential electrochemical mass spectroscopy measurements, X-ray absorption spectroscopy analysis and theoretical calculations indicate that OER reaction on Nb 0.1 Mn 0.1 Ru 0.8 O 2 primarily follows the adsorbate evolution mechanism with much favorable energy barrier accompanied by a locally passivated lattice oxygen mechanism (AEM-LPLOM) and the co-existed Nb and Mn in RuO 2 crystal lattice could not only stabilize the lattice oxygen, but also relieve the valence state fluctuation of Ru site to stabilize the catalyst during the reaction.
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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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）