Journal of Energy Chemistry
·
2024
·
IF 14
Yunbo Li,Jianchao Yue,Chaoyi Yang,Hongnan Jia,Hengjiang Cong,Wei Luo
Metastable nanostructured electrocatalyst with a completely different surface environment compared to conventional phase-based electrocatalyst often shows distinctive catalytic property. Although Ru-based electrocatalysts have been widely investigated toward hydrogen oxidation reaction (HOR) under alkaline electrolytes, these studies are mostly limited to conventional hexagonal-close-packed ( hcp ) phase, mainly arising from the lack of sufficient synthesis strategies. In this study, we report the precise synthesis of metastable binary RuW alloy with face-centered-cubic ( fcc ) phase. We find that the introduction of W can serve as fcc phase seeds and reduce the formation energy of metastable fcc -RuW alloy. Impressively, fcc -RuW exhibits remarkable alkaline HOR performance and stability with the activity of 0.67 mA cm Ru −2 , which is almost five and three times higher than that of hcp -Ru and commercial Pt/C, respectively, which is attributed to the optimized binding strength of adsorbed hydroxide intermediate derived from tailored electronic structure through W doping and phase engineering. Moreover, this strategy can also be applied to synthesize other metastable fcc -RuCr and fcc -RuMo alloys with enhanced HOR performances.
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
·
2025
·
IF 16
Hanjun Li,Fulin Yang,Guanghua Wang,Liheng Guan,Feili Lai,Nan Zhang,Tianxi Liu
The development of efficient electrocatalysts for alkaline hydrogen oxidation reaction (HOR) is essential for anion exchange membrane fuel cells and advancing the hydrogen economy. Herein, we demonstrated PtRuRhPdIr high-entropy alloy aerogels (HEAAs) with highly distorted structure as efficient HOR electrocatalysts and realized effective control of PtRu-based metallic aerogels (MAs) with elemental components ranging from two to seven. Specially, PtRuRhPdIr HEAAs on carbon (PtRuRhPdIr HEAAs/C) exhibit excellent HOR activity, with Pt group metal (PGM)-normalized mass activity (5.75 A mgPGM–1) at 50 mV and exchange current density normalized by electrochemical surface area (0.69 mA cm–2), approximately 16.9 and 4.1 times that of the commercial Pt/C (0.34 A mgPGM–1, 0.17 mA cm–2), respectively. The mechanism study shows that the highly distorted PtRuRhPdIr HEAAs provide abundant unsaturated sites for HOR, and the synergistic effect of multiple-active sites balances the adsorption of H* and *OH, boosting the HOR performance.
研究领域:
材料科学
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能源化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoning Wang,Xuejin Li,Tonghui Cai,Yongpeng Cui,Dongqing Kong,Jing Xu,Haoyu Hu,Yesheng Wang,Han Hu,Xiuli Gao,Yanpeng Li,Qingzhong Xue,Zifeng Yan,Lianming Zhao,Wei Xing
Designing electrocatalysts for hydrogen oxidation reaction (HOR) in alkaline media is crucial but challenging. Among all available electrocatalysts, Ni-based materials are recognized as the most potential precious-metal-free electrocatalysts for HOR. However, they still suffer from serious problems including low activity and poor stability. In this work, a synergistic chemical anchoring and electronic structure regulation strategy is proposed to gain both high electrocatalytic activity and stability for Ni-based HOR catalyst. N-doped graphite nanoflakes (N-GFs) support with abundant N anchoring sites can stabilize the loading of Ni-based active species, giving rise to an excellent stability of the catalyst. Meanwhile, the rationally designed heterostructure in the active Ni 3 N/Ni can trigger the electron transfer across the heterointerface, which optimizes the binding energy of the reaction intermediates, resulting in an accelerated the Volmer reaction. Benefited from the rational design, Ni 3 N/Ni/N-GFs exhibits excellent mass activity (42.7 A g Ni -1 at the overpotential of 50 mV) and stability (more than 24 h continuous operation). Moreover, the Ni 3 N/Ni heterostructure performs better in HOR electrocatalysis than individual Ni or Ni 3 N. These experimental results are rationalized by the theoretical simulations, which demonstrate that the heterostructure effectively weakens the hydrogen adsorption, optimizes the hydroxyl adsorption, and decreases the water formation reaction barrier.
研究领域:
材料科学
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电催化
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 28
·12064-12070
·
IF 6.7
Hai Liu,Zhuang Zhang,Mengxuan Li,Yaping Li,Yun Kuang,Xiaoming Sun
Developing highly efficient hydrogen oxidation reaction (HOR) electrocatalysts in alkaline media is of great significance for anion exchange membrane fuel cells (AEMFCs). Herein, we report an efficient Ru-doped hexagonal tungsten trioxide (Ru-WO3) HOR electrocatalyst through a hydrothermal strategy. The prepared Ru-WO3 electrocatalyst exhibits enhanced HOR performance with a 6.1 times higher exchange current density and better durability than commercial Pt/C. Structural characterizations and theoretical calculations reveal that the uniformly distributed Ru was modulated by oxygen defects and the electron transfer from O to Ru modulated the H* adsorption of Ru sites. In addition, plenty of W sites can serve as hydroxyl adsorption sites to accelerate the HOR kinetics. This work not only provides an efficient HOR catalyst in alkaline media, but also promotes the fundamental understanding of the effect of modulation on the adsorption of H* and *OH in tungsten oxides with a relatively low oxidation state by Ru doping, broadening the range of HOR catalysts to Ru-doped metal oxides.
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
JOURNAL OF CATALYSIS
·
2020
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IF 7.888
Guoju Huang,Wanli Liang,Yinlong Wu,Jiawang Li,Yan Qi Jin,Hongbin Zeng,Hao Zhang,Fangyan Xie,Jian Chen,Nan Wang,Yanshuo Jin,Hui Meng
Due to the rapid development of alkaline polymer electrolyte fuel cells and water splitting, it is becoming increasingly urgent to develop non-precious metal electrocatalysts for the hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) in alkaline medium. Herein, Co 2 P/CoP hybrid is synthesized from cobalt carbonate hydroxide (CoCH) precursor, and further evaluated for the electrocatalytic HOR and HER in alkaline electrolytes. Specifically, benefiting from the reasonable hybrid structure that integrate suitable hydrogen adsorption energy of CoP and excellent conductivity of Co 2 P, Co 2 P/CoP hybrid exhibits excellent catalytic activities. The Co 2 P/CoP@NF hybrid has impressive HER activity, with a current density of −10 mA cm −2 at the overpotentials of −61 mV and the Tafel slope of 55.1 mV dec −1 , which can compete with recently reported transition metal phosphides and cobalt-based catalysts. In addition, the exchange current density of Co 2 P/CoP@NF hybrid is ~ 0.82 mA cm −2 for HOR, which is close to commercial Pt/C catalyst (~1.14 mA cm −2 ).
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuanyuan Cong,Mengling Liu,Luyun Chen,Yurong Qi,Limin Zhang,Qiuping Zhao,Chunlei Li,Haibin Wang
The sluggish hydrogen energy conversion kinetics in alkaline medium and the complete passivation under high anodic potential as well as the easy detachment of active sites from the carbon substrate are three critical challenges of Ru-based electrocatalysts for their practical application. Herein, Ru (single atoms and nanoclusters)-embedded TiO 2-x (Ru SA -Ru NC /TiO 2-x ) well solves above-mentioned urgent problems simultaneously. Specifically, the optimal Ru SA -Ru NC /TiO 2-x electrocatalyst delivers a mass activity of 1620 A g Ru –1 and a low overpotential of 24 mV at 10 mA cm −2 in alkaline hydrogen oxidation and evolution reactions (HOR/HER), respectively. More importantly, the Ru/TiO 2-x can unprecedentedly catalyze the HOR up to a potential of 1.2 V vs. RHE without deactivation and almost maintain unchanged after accelerated stability tests of 10,000 CVs or the presence of 100 ppm CO impurity. Confirmed by in/ex-situ experimental measurements and computational analyses, the enhancement in performance is attributed mainly to the construction of high-density Ru-Ti bonds, maintaining the unblocked charge transfer from TiO 2 to Ru and achieving more low-valence Ru species. The observed Ti 3+ species on oxygen vacancies derived from the original structure and in-situ formation during the electrochemical reaction would be preferentially oxidized, further protecting Ru sites and aiding in the electrocatalytic process. Benefiting from Ru-Ti bonds and triggered oxygen vacancies, Ru could serve as exclusive optimal H adsorption sites and cooperate with the OH ad on Ti sites, rapidly and stably accelerating hydrogen energy conversion.
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
Advanced Sustainable Systems
·
2025
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IF 6.1
Chunxia Wu,Fangpu Zhang,Tao Sun,Zhixue Zhang,Junlin She,Zerui Mu,Zhaoyu Wang,Yuening Liang,Zhaojun Liu,Chuanbo Gao
High-entropy alloy nanowires (HEA NWs) hold significant promise for achieving exceptional catalytic activity and stability, owing to their unique 1D morphology and the electronic engineering potential of the HEAs. However, the controlled synthesis of HEA NWs remains a challenge. In this work, a novel wet-chemical approach is reported for the synthesis of ultrathin HEA NWs, represented by PtRuNiCuPb, through an active-hydrogen (H·)-mediated reduction mechanism. The H· species, generated by organic dehydrogenation, facilitate the effective co-reduction of metal salts with differing reduction potentials, while the mild synthesis conditions ensure morphology control toward nanowire formation. The resulting PtRuNiCuPb HEA NWs exhibit remarkable catalytic activity in electrocatalytic hydrogen oxidation reaction (HOR) in alkaline media, due to their multimetallic compositions and abundant grain boundaries. At 50 mV, the specific and mass activities reach 8.46 mA cm −2 and 5.54 A mg Pt+Ru −1 , respectively, ≈11.3 and 14.5 times greater than those of commercial Pt/C. Thanks to the unique 1D morphology, the PtRuNiCuPb HEA nanowires demonstrate excellent catalytic stability, retaining 97% of their initial mass activity after 20000 cycles of accelerated durability testing. These findings offer a promising strategy for designing highly efficient and durable catalysts using HEA compositions and 1D morphologies for electrocatalytic applications.
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
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Peng Wang,Hao Cui,Chengxin Wang
Although Pt-based alloy catalysts have been considered promising candidates for fuel cell applications, constructing highly efficient, multifunctional Pt-based catalysts that simultaneously boost the three key reactions (MOR, ORR and HOR) in proton exchange membrane fuel cells (PEMFCs) remains a huge challenge. Herein, PtMo-CeO x hybrids with interesting ultrathin and ultralong nanowire assemblies (NAs) structure are synthesized by a one-pot solvothermal method without templates. The PtMo-CeO x -NAs catalyst exhibits 5.2-fold, 6.9-fold and 2.4-fold higher mass activity than commercial Pt/C towards the MOR, ORR and HOR simultaneously and shows excellent durability and CO poisoning tolerance. Detailed experiments reveal that the enhancement should be due to strain and ligand effects. Most impressively, when PtMo-CeO x -NAs membrane electrode assemblies (MEAs) fabricated by a catalyst-coated method are used both as the anode and cathode in PEMFCs, the performance of fuel cells is dramatically boosted compared to those with Pt/C.
研究领域:
材料科学
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催化化学
·
燃料电池研究
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Wang Xiaoning,Tong Yanfu,Feng Wenting,Liu Pengyun,Li Xuejin,Cui Yongpeng,Cai Tonghui,Zhao Lianming,Xue Qingzhong,Yan Zifeng,Yuan Xun,Xing Wei
Designing Pt-based electrocatalysts with high catalytic activity and CO tolerance is challenging but extremely desirable for alkaline hydrogen oxidation reaction. Herein we report the design of a series of single-atom lanthanide (La, Ce, Pr, Nd, and Lu)-embedded ultrasmall Pt nanoclusters for efficient alkaline hydrogen electro-oxidation catalysis based on vapor filling and spatially confined reduction/growth of metal species. Mechanism studies reveal that oxophilic single-atom lanthanide species in Pt nanoclusters can serve as the Lewis acid site for selective OH - adsorption and regulate the binding strength of intermediates on Pt sites, which promotes the kinetics of hydrogen oxidation and CO oxidation by accelerating the combination of OH − and *H/*CO in kinetics and thermodynamics, endowing the electrocatalyst with up to 14.3-times higher mass activity than commercial Pt/C and enhanced CO tolerance. This work may shed light on the design of metal nanocluster-based electrocatalysts for energy conversion.
研究领域:
材料科学
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电化学
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能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 46
·26323-26329
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IF 12.732
Wangjin Ji,Changhong Zhan,Deyu Li,Yong Xu,Ying Zhang,Lu Wang,Liangbin Liu,Yu Wang,Wenxing Chen,Hongbo Geng,Xiaoqing Huang
The hydrogen oxidation reaction (HOR) has recently attracted great attention, yet the poor performance of HOR over the platinum group metal-free (PGMs-free) catalysts in alkaline conditions strongly impedes the development of hydroxide-exchange membrane fuel cells. Here, we demonstrate that the phase and interface engineering of nickel carbide (Ni3C) nanobranches can significantly enhance the alkaline HOR performance. Specifically, such interface engineering is realized through a facile annealing treatment of a branched Ni3C nanostructure. As a promising PGMs-free HOR catalyst, the strong interfacial synergy of Ni/Ni3C significantly enhances the HOR performance in alkaline media, with the HOR activity being comparable to that of a commercial Pt/C catalyst, and it demonstrates excellent CO tolerance. Mechanism studies show that the interfacial synergy facilitates electron transfer from Ni to Ni3C and thus regulates the absorption strengths of *H and *OH. This work opens up a new avenue for the design of high-performance PGM-free catalysts for electrocatalysis and beyond.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yonghuan Li,Guang Jiang,Yue Yang,Wei Song,Hongmei Yu,Jinkai Hao,Zhigang Shao
Cell reversal has a significant impact on the durability of proton exchange membrane fuel cell (PEMFC). Oxygen evolution reaction (OER) catalysts are often introduced to serve as reversal tolerant materials. However, adding OER catalysts to the anode may lead to a reduction in performance as they could potentially cover the active Pt site. In this study, carbon nanotube (CNT) supported Pt-Ir bifunctional catalyst is used as the anode catalyst to balance the tradeoff between cell reversal resistance and power generation performance. The obtained Pt 3 Ir 1 /CNT catalyst exhibits a faster OER kinetic (83.8 mV dec −1 ) than the commercial Pt/C (151.8 mV dec −1 ) catalyst and the similar hydrogen oxidation reaction (HOR) activity with Pt/C. After the accelerated durability test, the electrochemical active surface area (ECSA) loss of Pt 3 Ir 1 /CNT is 19.6% while that of Pt/C is 54.7%. After 50 consecutive cell reversal tests, it was observed that the MEA with Pt 3 Ir 1 /CNT exhibits almost no degradation in cell voltage . In contrast, the MEA with Pt/C showed a degradation of 4.9% (@ 1000 mA cm −2 ) when subjected to the same conditions. The strategy of combing bifunctional catalysts with high-durability supports has been shown to improve the reversal tolerance of the cell without performance loss.
研究领域:
能源材料科学
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电化学
✓ 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）