JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
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IF 8.128
Yanshan Mo,Shouquan Feng,Tianqi Yu,Jinli Chen,Guangfu Qian,Lin Luo,Shibin Yin
PtNi alloy nanoparticles display promising catalytic activity for oxygen reduction reaction (ORR), while the Ostwald ripening of particles and the dissolution/migration of surface atoms greatly affect its stability thus restricting the application. Herein, the WO x -surface modified PtNi alloy nanowires (WO x -PtNi NWs) exhibiting enhanced ORR catalytic property is reported, which has high aspect ratio with the diameter of only 2 ∼ 3 nm. It is found that the WO x -PtNi NWs shows a volcano relationship between the ORR activity and the content of WO x . The WO x-(0.25) -PtNi NWs has the best performance among all the synthesized catalysts. Its mass activity (0.85 A mg −1 Pt ) is reduced by only 23.89% after 30k cycles durability test, which is much more stable than that of PtNi NWs (0.33 A mg −1 Pt , 45.94%) and Pt/C (0.14 A mg −1 Pt , 57.79%). Hence this work achieves an effective regulation of the ORR activity for PtNi alloy NWs by the synergistic effect of WO x on Pt.
研究领域:
催化
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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
FUEL
·
2025
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IF 7.5
Wenji Liang,Junwei Shi,Zhenhua Qin,Jinguang Cai,Yun He,Jianfen Li
Exploring efficient and durable non-noble metal catalysts toward oxygen reduction/evolution reaction (ORR/OER) is of practical significance in advancing Zn-air batteries. Herein, we introduce a three-dimensional (3D) bifunctional electrocatalyst (Fe/Ni@NSC) consisting of N, S-dual doped mesoporous carbon nanosheets/carbon nanotubes embedded with abundant FeS/FeNi nanoparticles and Fe/Ni-N x sites by integrating rod-like ZIF-L@S-g-C 3 N 4 with Fe/Ni-phen complex and subsequent pyrolysis. The 3D structure not only offers a high surface area for active sites but also accelerates O 2 transport/charge transfer. Leveraging the synergistic effect of the 3D porous carbon network and multiple active sites, Fe/Ni@NSC exhibited outstanding activities in both ORR (half-wave potential, 0.868 V) and OER (overpotential, 317 mV at 10 mA cm −2 ), indicating a low potential gap of 0.679 V, outperforming the Pt/C + RuO 2 benchmarks (0.695 V). The Zn-air batteries based on Fe/Ni@NSC achieved a promising open circuit voltage (1.47 V), peak power density (172.59 mW cm −2 ), as well as long-term cycling stability (370 h). Furthermore, density functional theory (DFT) calculations also demonstrated that the interfacial electronic interaction between FeS and FeNi effectively boosted the bifunctional catalytic performance for ORR/OER. This study lays the foundation for designing low-cost and efficient 3D structure non-noble metal catalysts for more energy conversion and storage devices.
✓ 已验证
产品关联
DOI
高影响因子
Scientific Reports
·
2025
·Vol. 15
·期 1
·1-11
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IF 3.9
Jin Hong,Lin Dejian,Zhou Laihong,Zha Guojun,Wu Huanwen,Li Shuigen,Jiang Minhua,Huang Ping,Xie Haijiao
Electrocatalytic materials with dual functions of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have received increasing attention in the field of zinc-air batteries (ZABs) research. In this study, bifunctional CoNC@NCXS catalysts were prepared by anchoring Co and N co-doped CoNC on N-doped carbon xerogel sphere (NCXS) based on the spatially confined domain effect and in-situ doping technique. CoNC@NCXS exhibited excellent ORR/OER activity in alkaline electrolytes with the ORR onset potential of 0.99 V, the half-wave potential (E 1/2 ) of 0.78 V at 10 mA cm −2 and the OER overpotential of 360 mV at 10 mA cm −2 . These excellent catalytic activities were derived from constructing composite active structures and enhancing electrocatalytic efficiency. The ZAB assembled with CoNC@NCXS catalyst had a discharge specific capacity of 710 mAh g −1 at a current density of 10 mA cm −2 , which was superior to that of the Pt/C&RuO 2 catalyst-assembled battery (667 mAh g −1 ). After running for 150 h, the charge and discharge efficiency of the CoNC@NCXS battery decreased by only 12.8%, which confirmed the excellent stability of the CoNC@NCXS catalyst. The free energy diagrams showed that, CoNC@NCXS has lower energy barriers and higher potential than CoNC in key reaction steps. This study provides a new perspective for the structural design of highly active composite catalysts in energy storage and conversion.
研究领域:
材料科学
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能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE CHEMICAL LETTERS
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2023
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IF 9.1
Yifen He,Chao Qu,Na Ren,Dawei Liang
ABSTRACT Recently, a novel 2-electron oxygen reduction reaction (ORR) based electro-oxidation (EO) system was developed, which utilizes a H 2 O 2 generation cathode instead of H 2 evolution cathode. A Ti-based Ni-Sb co-doped SnO 2 (Ti/NATO) anode was selected for efficient degradation of refractory organics and O 3 production. The synergistic reaction of O 3 /H 2 O 2 further accelerated the generation of hydroxyl radicals ( • OH) in the ORR-EO system. However, the catalytic activity and long-term effectiveness of the Ti/NATO anode limited the large-scale application of the ORR-EO process. In this study, a blue TiO 2 nanotube array (blue-TiO 2 -NTA) inter-layer was introduced into the fabrication process between the Ti substrate and NATO catalyst layer. Compared to the Ti/NATO anode, the Ti/blue-TiO 2 -NTA/NATO anode achieved higher efficiency of organic removal and O 3 generation. Additionally, the accelerated lifetime of the Ti/blue-TiO 2 -NTA/NATO anode was increased by 7 times compared to the Ti/NATO anode. When combined with CNTs-C/PTFE air cathode in ORR-EO system, all anodic oxidation and O 3 /H 2 O 2 processes achieved higher • OH production. Over 92% of TOC in leachate bio-effluent was effectively eliminated with a relatively low energy cost of 45 kWh/t.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2022
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IF 6.959
Jiao Xie,Yi Wang,Guichan Chen,Dengjie Chen
Oxygen electrocatalysts are crucial for the development of renewable and sustainable energy conversion/storage (ECS) systems, but a shortage of efficient and low-cost oxygen electrocatalysts is impeding their widespread applications. In this work, to investigate the bifunctionality of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), Ni-substituted LaMnO3 perovskite oxides (LaNixMn1–xO3, x = 0.1, 0.3, 0.5, 0.7, and 0.9) and pristine LaNiO3 and LaMnO3 were synthesized using a sol–gel process. After the compositional optimization and electrochemical characterizations, we identified that LaNi0.3Mn0.7O3 (SG LNM-3) within the compositions exhibited balanced intrinsic activity for bifunctional ORR and OER. To further improve the apparent activity of the optimized SG LNM-3, electrospinning was used to prepare one-dimensional nanostructured LaNi0.3Mn0.7O3 (ES LNM-3). ES LNM-3 had a higher specific surface area and continuous electron-transfer pathways, resulting in much improved bifunctional activity in comparison to SG LNM-3. In addition to the morphological effect, we ascribed the high electrochemical performance of ES LNM-3 to the high-spin Mn3+ and low-spin Ni3+ with electron configurations of t2g3eg1 and t2g6eg1 (a well-recognized design descriptor), as well as the high degree of Jahn–Teller distortion. After assembling ES LNM-3 within Zn–air batteries, promising electrochemical performances such as high power density and rate capability were obtained. Our findings will advance the development of high-performance and inexpensive oxygen electrocatalysts and associated ECS devices.
研究领域:
材料科学
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电化学
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能量转换与存储
✓ 已验证
DOI
高影响因子
International Journal of Electrochemical Science
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2023
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IF 1.5
Qijian Niu,Oluwafunmilola Ola,Nannan Wang,Binling Chen,Yanqiu Zhu,Yongde Xia
In this work, Co 9 S 8 and N,S co-dopped carbon encapsulated WS 2 nanocomposites (Co 9 S 8 -N,S-C@WS 2 ) has been successfully prepared through a high-temperature carbonization of the precursor ZIF-67@WS 2 nanoparticles. The obtained Co 9 S 8 -N,S-C@WS 2 nanoparticles were confirmed to have a core-shell structure and uniform element distribution by TEM and element mapping. Its crystal structure was characterized by XRD, and the high specific surface areas with porous structure was characterized by BET tests. The as-prepared Co 9 S 8 -N,S-C@WS 2 nanoparticles exhibited a better ORR/OER/HER performance than single component. In this work, a novel idea for the preparation of functional nanocomposite materials could be provided.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Zhou Wanlin,Su Hui,Cheng Weiren,Li Yuanli,Jiang Jingjing,Liu Meihuan,Yu Feifan,Wang Wei,Wei Shiqiang,Liu Qinghua
The electrochemical oxygen reduction reaction (ORR) is at the heart of modern sustainable energy technologies. However, the linear scaling relationship of this multistep reaction now becomes the bottleneck for accelerating kinetics. Herein, we propose a strategy of using intermetallic-distance-regulated atomic-scale bimetal assembly (ABA) that can catalyse direct O‒O radical breakage without the formation of redundant *OOH intermediates, which could regulate the inherent linear scaling relationship and cause the ORR on ABA to follow a fast-kinetic dual-sites mechanism. Using in situ synchrotron spectroscopy, we directly observe that a self-adjustable N-bridged Pt = N 2 = Fe assembly promotes the generation of a key intermediate state (Pt‒O‒O‒Fe) during the ORR process, resulting in high reaction kinetics and selectivity. The well-designed Pt = N 2 = Fe ABA catalyst achieves a nearly two orders of magnitude enhanced kinetic current density at the half-wave potential of 0.95 V relative to commercial Pt/C and an almost 99% efficiency of 4-electron pathway selectivity, making it one of the potential ORR catalysts for application to the energy device of zinc‒air cells. This study provides a helpful design principle for developing and optimizing other efficient ORR electrocatalysts.
研究领域:
电化学
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材料科学
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催化
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可持续能源
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
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2024
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IF 8.9
Jizhao Zou,Tao Liang,Minggui Peng,Peng Liu,Zhe Li,Jiaming Wen,Zhangjian Li,Yusheng Yan,Xin Yu,Xierong Zeng,Junfeng Huang
Integration of cations doping by using unpaired high-spin electrons through the valence state substitution is deemed as a prospective strategy for construction of oxygen vacancies, regulation of inner electronic structures and enhancement of surface properties. Herein, an effective strategy is proposed to construct massive oxygen vacancies into 2D nitrogen-doped carbon nanosheets by the design of heterogeneous interfaces between CoFe alloy and CoFe 2 O 4 nanoparticles. The valence state transition for Fe and Co endows electronic transfer capability and charge density around the oxygen atoms. The prepared CoFe-CoFe 2 O 4 @NCs-4 catalyst exhibits maximum content of oxygen vacancies (Density of O vac 50.1 %). It shows excellent ORR activity with a half-wave potential of 0.83 V and OER overpotential of 320 mV. Reversible Zn-air batteries assembled by the CoFe-CoFe 2 O 4 @NCs-4 catalysts exhibit a power density of 106.32 mW cm −2 and durable stability (500 h at the current density of 10 mA cm −2 ), which also are superior to those of the commercial 20 wt% Pt/C + RuO 2 catalyst. The excellent bifunctional catalytic performance can be attributed to synergistic effects between massive oxygen vacancies, ultrahigh specific surface area (545.9 m 2 g −1 ) and heterogeneous interfacial structure. This work provides valuable insight into designing efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Sun Yining,Fan Kui,Li Jinze,Wang Lei,Yang Yusen,Li Zhenhua,Shao Mingfei,Duan Xue
The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O 2 ) is appealing due to its sustainability. However, its efficiency is compromised by the competing 4e − ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with a single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. The electrode exhibits excellent 2e − ORR performance under alkaline conditions and achieves H 2 O 2 yield rates of 0.73 mol g cat −1 h −1 in the H-cell and 5.48 mol g cat −1 h −1 in the flow cell, outperforming most reported catalysts. The experimental results show that the Ni atoms selectively adsorb O 2 , while carbon nanosheets generate reactive hydrogen species, synergistically enhancing H 2 O 2 production. Furthermore, a coupling reaction system integrating the 2e − ORR with ethylene glycol oxidation significantly enhances H 2 O 2 yield rate to 7.30 mol g cat −1 h −1 while producing valuable glycolic acid. Moreover, we convert alkaline electrolyte containing H 2 O 2 directly into the downstream product sodium perborate to reduce the separation cost further. Techno-economic analysis validates the economic viability of this system.
研究领域:
电化学
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催化
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材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Shengzhi He,Jingyu Wang,Chunwen Sun
Oxygen reduction reaction (ORR) serves as the foundation for various electrochemical energy storage devices. Fe/N C catalysts are expected to replace commercial Pt/C as oxygen electrode catalysts based on the structural tunability at the atomic level, abundant iron ore reserves and excellent activity. Nevertheless, the lack of durability and low active site density impede its advancement. In this work, a durable catalyst, Cu Fe/N C, for ORR was prepared by modulating the interfacial composition and electronic structure. The introduction of Cu nanoclusters partially eliminates the Fenton effect from Fe and optimizes the electron structure of Fe N x , thereby effectively enhancing the long-term durability and activity. The prepared Cu Fe/N C exhibits a half-wave potential ( E 1/2 ) of 0.90 V and superior stability with a decrease in E 1/2 of only 20 mV after 10,000 cycles. The assembled alkaline Zinc-Air batteries (ZABs) with Cu Fe/N C exhibit an open-circuit potential of 1.458 V. At a current density of 5 mA cm −2 , the batteries are capable of operation for 600 h with a stable polarization. This Cu Fe/N C may promote the practical application of novel and renewable electrochemical energy storage devices.
研究领域:
电化学
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催化
·
能量存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Ji Zhou,Chen Liu,Yifei Liao,Guanghui Xia,Qin Huang,Yisha Huang,Yigang Yan,Chaoling Wu,Yao Wang
Catalysts with a platinum-rich shell and intermetallic core are considered to be one of the most promising catalysts for the oxygen reduction reaction (ORR) in fuel cells. However, too thin of a platinum-rich shell makes the core–shell structure easy to lose. Therefore, the development of the core–shell structure with an appropriate thickness of platinum-rich shell and intermetallic core remains a huge challenge in the field of fuel cells. In this paper, PtCoN-1000/C catalyst with about 1 nm thick platinum-rich shell shows significantly enhanced ORR activity and stability in acidic electrolyte, which is superior to L10-PtCo/C and commercial Pt/C catalysts. The specific power at 0.8 V and mass activity at 0.9 V are 5.60 W mgPt–1 and 0.74 A mgPt–1, respectively. It suggests that the tensile strain and moderately thickened platinum-rich shell led by nitrogen doping can greatly improve the performance of the catalyst.
研究领域:
材料科学
·
电化学
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催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2020
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IF 8.821
Shuqi Hu,Wenpeng Ni,Daihui Yang,Chao Ma,Jiaheng Zhang,Junfei Duan,Yang Gao,Shiguo Zhang
Atomically dispersed Fe–N–C catalysts with additional Fe-containing nanoparticles including metal, carbides or oxides have shown great potentials towards oxygen reduction reaction (ORR) catalysis. However, the formation of these synergistically active nanoparticles and the effect of the porous carbon structures remain unclear. In this work, a novel single-atom-involved electrochemical catalyst, i.e. , Fe 3 O 4 nanoparticles encapsulated in atomically dispersed Fe–N–C (Fe 3 O 4 @FeNC) was reported. The optimized Fe 3 O 4 @FeNC exhibits excellent ORR activity with a half-wave potential of 0.890 V and a Tafel slope of 58.8 mV dec −1 , comparable with recently reported ORR catalysts and superior to these of commercial Pt/C. More importantly, the porous architectures not only affect the mass transfer and active sites, but casts huge influence on the nucleation of Fe 3 O 4 nanoparticles, the graphitization degree of the carbon support, the chemical environments of the elements, and the ORR catalytic pathways. Density functional theory calculations show stronger O 2 adsorption on Fe–N–C when supported on Fe 3 O 4 moieties, which may increase the reactant concentration for ORR and promote the overall activity. These findings will provide important references for the future understanding and design of single-atom-involved catalysts with enhanced electrochemical properties .
研究领域:
材料科学
·
电化学
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催化
·
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）