INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Zhaoying Yang,Xinge Wu,Gaowu Qin,Xiangying Meng
FeCo-N-C is considered a promising electrode material for hydrogen fuel cells. However, its oxygen reduction reaction (ORR) performance is limited by the strong adsorption of intermediates. In this work, we regulated the adsorption of “metal-intermediates” by modulating the interaction between the metal and support. The sulfur atoms were introduced to modify the periphery of the M-N x sites, and an atom-dispersed bimetallic site micro-mesoporous catalyst (FeCo-SN-C) was synthesized. The S dopant enhances the bonding between the metal catalytic sites and the support, which weakens the adsorption of ORR intermediates on catalytic sites, resulting in exceptional stability and ORR activity of the catalyst. ORR tests showed that FeCo-SN-C in 0.1 M KOH exhibited superior half-wave potential (0.863 V vs. RHE), which outperformed Pt/C (0.833 V), along with high stability and methanol tolerance. Theoretical calculations demonstrated that the doping of S effectively shifted the 3d electron orbital of the Fe site to a deeper level, optimized the adsorption and desorption energy barriers of the key oxygen-containing intermediate (∗OH), and promoted the ORR. Additionally, the Zn-air batteries based on FeCo-SN-C exhibited excellent discharge performance and durability. This study provides insights and solutions for the rational design of TM-N-C catalysts to enhance their activity and stability.
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
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yingchao Wang,Jingjing Wu,Xianglong Lu,YuMin Guo,Huining Zhao,Xin Tang
The bifunctional catalysts which can improve both oxygen evolution (OER) and oxygen reduction reaction (ORR) activity are highly desirable for fuel cells, metal-air batteries and water splitting. Here, we report a perovskite structure Sr 0.9 M 0.1 RuO 3-δ (SMRO, M=K, Na, Ag) synthesized via sol-gel method performing excellent bifunctional catalytic activity. With the metal ion (M + ) doping in A-site, X-ray photoelectron spectroscopy analysis reveals that oxygen vacancy and lattice oxygen are introduced into the structure, which is confirmed as the primary reason for the improvement of catalytic activity. The highest OER and ORR activity among these four samples is observed in Sr 0.9 Ag 0.1 RuO 3 (SARO). This work may shed light on the designing of high-efficiency bifunctional OER/ORR electrocatalysts .
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 16
·6126-6132
·
IF 8.307
Jiawen Li,Peng Liu,Jianxin Mao,Jianyue Yan,Wenbo Song
Woven covalent organic frameworks (COFs) possess three-dimensional (3D) frameworks with well-dispersed variable metal centers, showing great promise in heterogeneous catalysis. Until now, woven COFs have not been exploited as catalysts. Herein, COF-112 (a typical woven COF) is utilized as an ORR catalyst to reveal the role of the metal center and linkage. Through metal center variation, the optimal COF-112Co with imine linkage exhibits superior ORR activity (Eonset = 0.87 V vs. RHE, n = 3.86, and JL = 5.78 mA cm−2). Experimental and theoretical studies demonstrate the non-metallic ORR active site and confirm the influence of metal variation in COF-112. A linkage conversion strategy reveals the importance of the imine linkage on the 4e− ORR. This work reveals the structure–activity relationship of woven COFs, which will broaden the application of COFs and extend the diversity of electrocatalysts.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 8
·3381-3393
·
IF 3.5
Zhang Feng,Wang Hao
Exorbitant cost and limited availability of platinum-based electrocatalysts for the oxygen reduction reaction (ORR) in metal–air batteries and alkaline fuel cells pose significant obstacles to the large-scale commercialization of these clean-energy technologies. Herein, we employed a cost-effective and sustainable bacterial cellulose biomass as the precursor to prepare a nitrogen and fluorine codoped metal-free ORR electrocatalyst (BCC-NF-900) by direct pyrolysis regulation. The BCC-NF-900 inherited the three-dimensional framework of bacterial cellulose, exhibiting a robust porous structure with a Brunauer–Emmett–Teller surface area of 196.9 m 2 ·g −1 . The pyridinic N (0.6 at%) and semi-ionic F (0.34 at%) species formed in the inert sp2 carbon skeletons synergistically regulated the electron spin and charge density of the adjacent C atoms. Such rational combination of a rapid transport pathway and effective active site led to high ORR activity (onset potential 0.89 V vs. RHE), methanol resistance, and electrochemical stability (merely 6.9% current loss) in alkaline electrolyte. Importantly, compared to the mere F-doped BCC-F-900 (onset potential 0.82 V vs. RHE) and N-doped BCC-N-900 (onset potential 0.77 V vs. RHE) catalysts, the BCC-NF-900 catalyst exhibited a markedly enhanced ORR performance, as evidenced by the measured onset potential. This study provides an available reference for the design of efficient metal-free catalysts for ORR, presenting a promising alternative to Pt/C catalysts in metal–air batteries and alkaline fuel cells.
研究领域:
材料科学
·
电化学
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能源技术
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纳米技术
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ruiqi Guo,Zhenglong Fan,Qiwei Zhou,Mengjie Ma,Wenxiang Zhu,Fan Liao,Hao Yang,Jiajie Wang,Zhenhui Kang,Minqi Sheng
Iridium oxide (IrO 2 ) has traditionally been considered to exhibit limited oxygen-reducing capacity. An effective approach to improve the oxygen reduction reaction (ORR) activity in parent catalytic materials is through atomic intercalation. However, the challenge lies in achieving a delicate balance between high ORR activity, structural stability, and minimizing the use of precious metals. Herein, we fabricate 3R-phase iridium oxide (3R-IrO 2 ) with superior ORR activity by intercalating a tiny amount of Pt (3.6 wt% Pt) into the interlayers of 3R-IrO 2 (3.6 wt% Pt-3R-IrO 2 ). When employed as an acidic ORR electrocatalyst, 3.6 wt% Pt-3R-IrO 2 shows a high half-wave potential (E 1/2 ) of 0.92 V (vs. RHE) in O 2 -saturated 0.1 M HClO 4 electrolyte, much better than those of Pt/C (0.850 V), 3R-IrO 2 (0.616 V), and Pt nanoparticles on 3R-IrO 2 surface (3.6 wt% Pt@3R-IrO 2 ) (0.618 V) electrocatalysts. It achieves high mass activity of 0.170 A mg Ir −1 at the potential of 0.9 V, which is 5.5 and 11.3 times than that of Pt/C (0.031 A mg Ir −1 ) and 3.6 wt% Pt@3R-IrO 2 (0.015 A mg Ir −1 ), respectively. Density functional theory (DFT) calculations and experiment results co-jointly demonstrate that the active center of Pt-3R-IrO 2 is anchored to the activated Ir atoms of the 3R-IrO 2 rather than Pt atoms. The d -band center of Ir 5 d orbitals of Pt-3R-IrO 2 is simultaneously regulated, which optimizes the energy barrier of adsorption/desorption toward the ORR process. Intriguingly, the intercalation of Pt atoms into trigonal rhodium oxide (Tri-RhO 2 ) also activates the ORR activity of Rh, suggesting the universality of this strategy. This discovery may provide a new and general way for activation of ORR activity of other precious metal-intercalated nonprecious metal oxide electrocatalysts.
研究领域:
材料科学
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电化学
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催化
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
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
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
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
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS RESEARCH
·
2023
·Vol. 38
·期 9
·2359-2368
·
IF 2.7
Ma Junjie,Liu Hangcheng,Tao Zeyu,Liu Jianfeng,Yuan Binxia,Pan Weiguo,Shi Zhengrong
In order to reveal the relationship between the structure and the electrochemical oxygen reduction reaction (ORR) activity of different double transition metal decorated catalysts, three different double transition metal and N co-doped carbon material cathode catalyst materials (FeCo–NC, FeNi–NC and CoNi–NC) were prepared in this study. The FeCo–NC catalysts synthesised in this study still showed high ORR activity under alkaline conditions, with a half-wave potential of 0.783 V RHE , a mass activity (MA) of 11.36 A/g (0.77 V RHE ) and an ultimate current density of − 4.46 mA cm −2 ; after 30,000 cycles, the half-wave potential only decreased to 99.3% of the initial potential. Meanwhile, we employ MS to establish three different double transition metal and N co-doped graphene catalysts and to calculate and analyse their desorption properties, leading to the FeCo–NC material being the model with the highest ORR activity, which is consistent with the experimental results. Graphical Abstract
研究领域:
电化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
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
·
催化
·
能量转换与存储
·
纳米技术
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Wei-Chang Chen,Xiao-Shuang Guo,Ze-Yu Liu,Chuan-Qing Huang,Jian-Shan Ye,Hai-Yang Liu,Xin-Yan Xiao
Fe-based nanoparticles encapsulated in carbon can effectively promote the ORR activity of the neighboring Fe–N x and prevent the dissolution of metal nanoparticles to ensure the long-term durability of catalysts. Herein, we employed a facile two step pyrolysis strategy to construct “plane-active sites” structure, namely FeO y nanoparticles embedded in carbon were loaded on two dimensional (2D) porous carbon with exposed abundant Fe–N x active sites (FeOy@C/Fe-N x /C). The optimized FeO y @C/Fe-N x /C catalyst with low Tafel slope (48 mV dec −1 ) and nearly-four-electron selectivity (3.91–3.97) showed excellent performance towards ORR with a more positive shift of 15 mV of half-wave potential (E 1/2 = 0.856 V) than that of commercial Pt/C (E 1/2 = 0.841 V) in alkaline solution, and also had a superior long-term stability and methanol resistance as compared with commercial Pt/C. The excellent electrochemical performance of FeO y @C/Fe-N x /C can be attributed to FeO y @C structure, exposed abundant Fe–N x active sites and two dimensional porous carbon with a large specific surface area.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）