Science Bulletin
·
2023
·
IF 18.9
Quanjun Tang,Liang Bai,Chen Zhang,Rongwei Meng,Li Wang,Chuannan Geng,Yong Guo,Feifei Wang,Yingxin Liu,Guisheng Song,Guowei Ling,Haitao Sun,Zhe Weng,Quan-Hong Yang
A dissolved-oxygen seawater battery (SWB) can generate electricity by reducing dissolved oxygen and sacrificing the metal anode at different depths and temperatures in the ocean, acting as the basic unit of spatially underwater energy networks for future maritime exploration. However, most traditional oxygen reduction reaction (ORR) catalysts are out of work at such ultralow dissolved oxygen concentration. Here, we proposed that the electronic axial stretching of the catalyst is essentially responsible for enhancing the catalyst’s sensitivity to dissolved oxygen. By modulating the lattice of iron phthalocyanine (FePc) as a model catalyst, the unique electronic axial stretching in the z -direction of planar FePc molecules was realized to achieve a boosted adsorption and electron transfer and result in a much improved ORR activity in lean-oxygen seawater environment. The peak power density of a homemade SWB using a practical carbon brush electrode decorated by the FePc is estimated to be as high as 3 W L − 1 . These results provide inspiring insights into the interaction between the catalyst and complicated seawater environment, and propose the electronic axial stretching as an effective indicator for the rational design of catalysts to be used in extremely lean-oxygen environment.
研究领域:
材料科学
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电化学
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能源存储
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产品关联
DOI
PubMed
高影响因子
Energy & Environmental Science
·
2021
·Vol. 14
·期 12
·6455-6463
·
IF 38.532
Meiqi Zhao,Haoran Liu,Hongwei Zhang,Wen Chen,Hanqin Sun,Zhenhua Wang,Biao Zhang,Lin Song,Yong Yang,Chao Ma,Yunhu Han,Wei Huang
Developing a highly efficient, easy-to-fabricate and non-noble metal electrocatalyst is vital for the oxygen reduction reaction (ORR). Herein, we fabricate a single Fe site catalyst Fe1/d-CN by developing a double-layer MOF strategy. The Fe1/d-CN catalyst shows an excellent ORR activity in the pH-universal range, especially in alkaline electrolytes with a record-level half-wave potential of 0.950 V, exceeding those of almost all the reported non-noble electrocatalysts and the commercial Pt/C catalyst (0.863 V). Besides its exceptional ORR activity in alkaline electrolytes, it also exhibits comparable ORR activity to the commercial Pt/C catalyst in acidic and neutral electrolytes. We speculate that the sources of the excellent pH-universal ORR performance can be attributed to the regulation of the electronic structure of Fe centres and the excellent electron/proton transport capability that comes from the rich defects and hierarchical porous features of the Fe1/d-CN catalyst. More excitingly, the catalyst possesses remarkable durability, and exhibits a negligible decrease after 30k accelerated durability test (ADT) cycles in pH-universal media. The flexible quasi-solid-state alkaline rechargeable Zn–air batteries with the Fe1/d-CN catalyst as the cathode show superior performance such as a high OCV of 1.50 V and peak power density of 78.0 mW cm−2. Furthermore, the flexible quasi-solid-state neutral rechargeable Zn–air batteries also exhibited remarkable performance.
研究领域:
材料科学
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电化学
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能源科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2026
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IF 7.8
Xiaopeng Zhang,Lin Chen,Longzhu Li,Xiaoming Yan,Junjiang Bao,Ning Zhang,Gaohong He
The introduction of guest metal molecules into metal–organic frameworks (MOFs) is an outstanding method to prepare dual-atom catalysts (DACs) with good oxygen reduction reaction (ORR) activity. However, most of the MOF-derived dual-atom catalysts reported to date exhibit a microporous structure and, therefore, suffer from the underutilization of active sites and poor mass transfer. This study employed NH2-MIL-101 as a precursor to form defect-bearing mesoporous Fe-NC via one-step pyrolysis for adsorbing [Co(en)3]3+, followed by secondary pyrolysis to generate Fe–Co binuclear site catalysts. The mesopores of NH2-MIL-101 are beneficial to [Co(en)3]3+ introduction and can improve the mass transfer of the ORR. Furthermore, the elevated nitrogen content within the [Co(en)3]3+ complex facilitates the co-coordination of Fe and Co with nitrogen, thereby enhancing the formation of Fe–Co diatomic sites. As a result, the obtained FeCo-NC-40 catalyst showed excellent ORR performance with a half-wave potential of 0.915 V (vs RHE). In addition, the liquid-phase Zn–air battery employing FeCo-NC-40 as the cathode catalyst demonstrated a peak power density of 178.13 mW·cm–2 and achieved a discharge specific capacity of 806.13 mAh·g–1 at 10 mA·cm–2, and there was no significant decay in stability for 10 days of continuous cycling.
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhenfei Liu,Dingding Ye,Xun Zhu,Shaolong Wang,Yanan Zou,Linghan Lan,Rong Chen,Yang Yang,Qiang Liao
Non-precious metal materials are considered as the most promising catalysts for oxygen reduction reaction (ORR) due to their high catalytic activity, low cost, superior stability as well as good electrocatalytic selectivity. Here, in situ encapsulation of Co nanoparticles into N-doped porous carbon (Co@NPC) nanocages interconnected by carbonized multi-walled carbon nanotubes (C-MWCNTs) are prepared through direct carbonization of the MWCNTs-based ZIF-67 precursor. The obtained hybrid material (denoted as Co@NPC/C-MWCNTs) displays an excellent ORR performance with a half-wave potential of 0.79 V, effective four-electron transfer and superior formate-tolerance ability. The superior ORR activity of the Co@NPC/C-MWCNTs hybrids is mainly ascribed to the abundant catalytic active sites contributed by the Co@NPC nanocages, the high electrical conductivity and large specific surface area rooting in C-MWCNTs, and synergetic effects between Co@NPC nanocages and C-MWCNTs. The membraneless flexible direct formate fuel cell (DFFC) using Co@NPC/C-MWCNTs as the cathode catalyst delivers a peak power density of 4.32 mW cm −2 stably. Notably, the performance of the flexible DFFC can still maintain 90.9% of its initial value after repeated bending for 1000 times. Moreover, two flexible DFFCs connected in series mode can easily power some low-power electronics. The report not only opens a new door to design high-performance non-precious metal ORR catalysts for DFFCs, but also greatly boosts the development of flexible energy conversion and storage devices.
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
ChemElectroChem
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2017
·Vol. 5
·期 4
·717-721
·
IF 4.136
Sicong Chen,Yuanzhi Zhu,Danyun Xu,Wenchao Peng,Yang Li,Guoliang Zhang,Fengbao Zhang,Xiaobin Fan
Graphical Let's synergize ORR : A novel hybrid catalyst of Co 3 O 4 and covalent triazine framework (CTF) is prepared through the in situ growth of Co 3 O 4 nanoparticles on CTF by using a hydrothermal method. This novel oxygen reduction reaction (ORR) catalyst shows a synergistic catalytic effect as well as comparable activity to the commercial Pt/C ORR catalyst (see picture). The oxygen reduction reaction (ORR) is an important process in energy conversion and storage devices. Great efforts have been focused on developing efficient, durable, and low-cost non-Pt catalysts. In this study, a novel hybrid ORR catalyst of Co 3 O 4 and covalent triazine framework (CTF) was prepared through the in-situ growth of Co 3 O 4 nanoparticles on CTF by using a hydrothermal method. Systematical studies revealed that this hybrid catalyst not only has a synergistic catalytic effect in the ORR, but also has superior stability and better methanol resistance than commercial Pt/C catalysts.
研究领域:
材料科学
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催化
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能量转换与存储
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纳米技术
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电化学
✓ 已验证
DOI
高影响因子
FUEL
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2024
·
IF 6.7
Yuxi Sun,Chuangang Yao,Zhe Zhang,Baixi Xia,Haixia Zhang,Jingyi Ding,Li Zhang,Wenwen Zhang,Xiaoshi Lang,Kedi Cai
The sluggish of the oxygen reduction reaction (ORR) kinetics and the susceptibility to CO 2 interactions are major barriers to the widespread application of solid oxide fuel cells (SOFCs). In this study, a non-metal cation doping strategy was employed to enhance the ORR catalytic activity and CO 2 tolerance of SrFeO 3- δ cathode. SrFe 1- x P x O 3- δ (SFP x , x = 0, 0.05, 0.1, 0.15, 0.2) materials were synthesized by substituting phosphorus (P) for Fe in SrFeO 3- δ . The doping of P facilitated the formation of oxygen vacancies in SrFeO 3- δ , enhancing oxygen adsorption, dissociation, diffusion, and charge transfer processes, leading to a notable increase in ORR catalytic activity. At 800 ℃, the polarization resistance of SFP 0.15 was 0.08 Ω cm 2 , a reduction of 42.86 % compared to undoped SrFeO 3- δ . Additionally, SFP 0.15 achieved a peak power density of 749.36 mW cm 2 , representing a 91.99 % enhancement over SrFeO 3- δ . These findings suggest that non-metal cation doping is an effective approach to boost the performance of SrFeO 3- δ perovskite cathode.
研究领域:
材料科学
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电化学
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能源材料
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燃料电池
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Huajing Zhou,Huichang Dong,Jinghao Wang,Yuancai Chen
A novel controllable mesoporous core–shell microsphere (Co/Fe 3 O 4 @PZS) is synthesized by polycondensation, and used as ORR electrocatalyst in the heterogeneous electro-Fenton (hetero-EF) reaction. Characteristic analysis indicated that PZS offered massive reactive sites for anchoring Co ions on the shell. Heteroatom Lewis acidic active sites, related with pyridinic N (4.15%), P = N/P-N (6.46%) and S = O (3.19%) bonds, were formed through the replacement of C = C groups with the N-P-S doped at the shell, which benefited the activating/generating reactive oxygen species (ROS), and capturing/degrading the target pollutant substrates. Moreover, PZS shells prevent the nano-Fe 3 O 4 crystals in the core from direct contact with the solution, which would greatly improve the stability of electrode with almost no leaching of Fe/Co ions after six successive runs. Electrochemical experiments confirmed the accelerating electron transfers among ≡Fe II/III /≡Co II/III by the direct electric activation, as evidenced by the decreasing potential discrepancy (from 0.175 to 0.123 V) and sharply increasing ring current (from 35 to 200μA), markedly improved the ORR toward two-electron process (n = 2.01). ESR and radical scavenging experiments verified that •OH and 1 O 2 served as the main ROS in the Co/Fe 3 O 4 @PZS hetero-EF system. In addition to the two-electron reduction ( O 2 → H 2 O 2 → Â · O H ), O 2 could also be directly electro-activated to 1 O 2 via one-electron reduction ( O 2 → Â · O 2 - / Â · HO 2 - → 1 O 2 ). Additionally, the regenerating/reducing of ≡Fe III /Co III could get the electron directly from the cathode without excess consumption of H 2 O 2 , all these could eventually facilitate BPA degradation with lower energy consumption (1.318 kWh m −3 ). This study provides a reliable and facile route to prepare mesoporous core–shell microsphere, and developed as doped cathode in the field of electro-Fenton electrocatalysis process.
研究领域:
环境科学
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材料科学
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电化学
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催化
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Siyuan Sun,Kexin Wei,Fan Yang,Yang Sun,Junpu An,Yongfeng Li
Carbon-based catalysts with free-standing structure are essential for rechargeable zinc-air battery as electrodes, which can avoid the side effects brought by organic binder. However, the current preparation methods still can be improved for faster preparation process and morphology control. In this study, we reported a fabrication strategy of self-standing carbon catalyst loaded with Co 3 Fe 7 nanoparticles and carbon nanotube as air electrodes for liquid rechargeable zinc-air battery. With a rapidly prepared PAN film used as substrate, ZIF with both Fe and Co elements are loading as active site precursor, which a composite structure of Co 3 Fe 7 nanoparticles and carbon nanotube will form on the free-standing catalyst surface after the carbonization process. In this structure, the carbonated PAN film substrate will provide rich conductive paths to promote electron transfer during the reaction process, and the active sites on the surface can promote the contact between intermediates and active sites. The optimized catalyst FeCo@CP-1:1 has the best ORR/OER bifunctional catalytic activity, which exhibits a halfwave potential (E 1/2 ) of 0.89 V (vs. RHE) for the ORR and a potential of 1.47 V at a current density of 10 mA cm −2 (E 10 ) for the OER. It can be attributed to the excellent ORR catalytic activity of Co 3 Fe 7 nanoparticles and its reconstruction process in OER. Furthermore, FeCo@CP-1:1 exhibits a power density of 154 mW cm −2 and long cyclic stability in liquid ZABs application. This research lays a practical foundation for design and synthesis of free-standing carbon catalyst.
研究领域:
材料科学
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电化学
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纳米技术
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能量存储
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Jialu Wei,Jingyu Wang,Wei Zhang,Yuezhen Mao,Chunwen Sun
Graphical A ZAB with Co–N–C–PBMCRO cathodic catalyst achieves a remarkable cycling stability for 788 h. The perovskite Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) composite was constructed by in situ exsolved CoRu nanoparticles and Co–N–C with more exposing active sites. A conductive pathway for oxygen ions and electrons was built, thereby enhancing the electrochemical bifunctional properties. This rational design strategy shows great potential for facilitating synthesis of perovskite based catalysts for energy conversion and storage applications. Bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are essential components of rechargeable zinc-air batteries. In this study, we synthesized a Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) perovskite composite with in situ exsolved CoRu nanoparticles and Co–N–C, functioning as an efficient bifunctional electrocatalyst for zinc-air batteries. The in situ exsolution of CoRu nanoparticles from the perovskite oxide was facilitated by the reducing action of 2-methylimidazole (2-MIM). Concurrently, Co–N–C was used to decorate PBMCRO, forming a novel bifunctional composite electrode of Co–N–C–PBMCRO. The incorporation of CoRu nanoparticles introduces a significant number of electrochemically active oxygen vacancies in the perovskite matrix, enhancing ORR and OER performance. Additionally, the Co–N–C synergistically improves electrochemical activity while preserving the structural stability of the perovskite oxide. The prepared Co–N–C–PBMCRO catalyst demonstrates significantly enhanced bifunctional performance compared to the undecorated pristine perovskite Pr 0.5 Ba 0.5 MnO 3−δ (PBMO). The zinc-air battery with Co–N–C–PBMCRO catalyst achieve a peak power density of approximately 90 mW/cm 2 and exhibit remarkable cycling stability for 788 h. This study presents a novel and effective strategy to enhance the catalytic performance of perovskite-based air electrodes for rechargeable metal-air batteries.
研究领域:
材料科学
·
电化学
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能源存储与转换
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xinyi Li,Jingjing Liu,Qinghai Cai,Ziwang Kan,Song Liu,Jingxiang Zhao
Modulating the microenvironment of single-metal active sites holds excellent promises for developing highly efficiently oxygen electrocatalysts. Herein, by combining theoretical predictions and experiments, we reported a general strategy to engineer the electronic properties of iron-nitrogen-carbon (FeN 4 /C) catalysts via the incorporation of the boron (B) atom for achieving improved catalytic activity in oxygen electrocatalysis. Our theoretical results revealed that B modulation effectively tunes the d-band center of the iron (Fe) active site to optimize its adsorption strength with oxygenated species, greatly enhancing oxygen reduction reaction (ORR) and oxygen evolution reactions (OER) activity. Our experimental measurements then confirmed the above theoretical predictions: the as-synthesized B-doped FeN 4 /C (Fe-N 4 -B) material can perform as an eligible bifunctional catalyst for ORR and OER in alkaline media, and its catalytic activity even outperforms the commercial noble metal benchmarks. The present findings provide a promising strategy to further design the advanced catalysts for a wide range of electrochemical applications.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Ruoqi Zong,Xiaobing Wu,Sung Yul Lim,Yusheng Fang,Bareera Raza,Yujuan Lu,Youkun Tao,Jing Shao
This study presents a straightforward chemical approach to induce cationic surface defects on SrCoO 3-δ (SCO) perovskites by selectively etching a-site Sr elements on the surface. The modified SCO-30 catalyst from this method exhibits an optimized thickness of cobalt-rich amorphous layer enriched with oxygen vacancies. This modification enhances the trifunctional catalytic activity for oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER) in an alkaline electrolyte. Importantly, the perovskite's structure remains unchanged during the surface engineering process. These findings underscore cationic defect engineering as an effective strategy for the rational design of high-performance electrocatalysts, showcasing potential applications in diverse electrochemical processes.
研究领域:
材料科学
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电化学
·
催化
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Zhe Zhang,Chuangang Yao,Haixia Zhang,Yuxi Sun,Baixi Xia,Wanning Liu,Jingyi Ding,Li Zhang,Xiaoshi Lang,Kedi Cai
LiCoO2 is widely used in lithium-ion batteries. Innovatively, this study reveals that by employing a synergistic strategy of Li volatilization and anion doping, LiCoO2-based materials demonstrate exceptional performance as solid oxide fuel cell (SOFC) cathodes. At high temperatures, Li volatilization forms a Co3O4 phase. Concurrently, anionic doping is achieved by substituting F ions for O ions. The synergy of these two strategies increases the concentration of oxygen vacancies and the formation of heterogeneous interfaces, effectively enhancing the adsorption, dissociation, and diffusion rates of oxygen, thereby significantly improving the oxygen reduction reaction (ORR) of LiCoO2 (LCO). LCOF1 (LiCoO1.9F0.1+Co3O4) exhibits an oxygen diffusion coefficient (Dchem) and surface exchange coefficient (Kchem) of 8.85 × 10–5 cm2 s–1 and 7.61 × 10–3 cm s–1, respectively, which are 45% and 26% higher than those of undoped LCO. Furthermore, at 800 °C, LCOF1 achieves a PPD of 0.86 W cm–2 and an Rp as low as 0.012 Ω cm2, representing improvements of 110% in PPD and a reduction of 78.6% in Rp compared to LCO. These findings indicate that the synergistic effect of Li volatilization and F doping is an effective strategy for enhancing the performance of Li-containing cathodes, offering valuable perspectives for the development of high-performance SOFC cathodes.
研究领域:
材料科学
·
电化学
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能源材料
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燃料电池
·
陶瓷
✓ 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）