JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Yuting Meng,Junajuan Yin,Tifeng Jiao,Jiahui Bai,Lexin Zhang,Jingjing Su,Shufeng Liu,Zhenhua Bai,Meiwen Cao,Qiuming Peng
The exploitation of high-efficiency, inexpensive, as well as durable electrocatalysts for the oxygen reduction reaction (ORR) is of vital importance for a number of emerging technologies, such as fuel cells to counter energy and environment crises. Herein, we describe a novel approach for the synthesis of conducting electrocatalysts derived from copper/cobalt-containing polypyrrole (PPy) hydrogel. This strategy relies on a pervasive supramolecular way toward controlled in situ synthesis of one-dimensional nanostructured conductive hydrogels using a reasonable dopant counter ion , which is a disc-shaped liquid crystal molecule copper phthalocyanine- 3,4′,4″,4‴-tetrasulfonic acid tetrasodium salt (CuPcTs). The formation of supramolecular crosslinked PPy hydrogel allows for efficient and homogeneous incorporation of highly active Co ion . Moreover, Co nanoparticles are also formed and doped into the carbon layer after pyrolysis, which further enhance the electrochemical activities. The prepared catalysts show outstanding electrocatalytic activity for the ORR reaction and the reaction process obviously conformed to a four-electron reduction mechanism in the alkaline electrolyte . Given the uniform nanostructures in present hydrogels, it is accredited that such strategy can offer new approach in high active nonprecious-metal-based electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Applied Materials Today
·
2025
·
IF 6.9
Yunpeng Ju,Wenhao Huang,Zhen Gao,Mingquan Liu,Naibao Huang
Effective bifunctional electrocatalysts for Oxygen reduction reaction and Oxygen evolution reaction (ORR and OER) are key for fuel cells and water electrolysis. Co-based dodecahedral bifunctional catalysts, rich in Co-N, pyridinic nitrogen, and metallic cobalt nanoparticles, were synthesized by pyrolysis of ZIF-67. The obtained ZIF-67–6 catalyst showed an onset potential of 0.90 V, a half-wave potential of 0.83 V (vs. RHE), a limiting diffusion current density of 5.24 mA cm⁻² for ORR, and an overpotential of 1.50 V (vs. RHE) at 10 mA cm⁻² for OER. These values are comparable to those of commercial 20 % Pt/C (0.89 V onset potential, 0.83 V half-wave potential, and 4.27 mA cm⁻² limiting diffusion current density) and IrO₂ (1.53 V overpotential at 10 mA cm⁻²). The catalyst maintained 92.11 % of its current density after polarizing at 0.80 V for 10,000 s. ZIF-67–6′s high performance and stability are attributed to the porous structure from MOF pyrolysis, the deposited cobalt nanoparticle, and the higher Co-N and the pyridinic nitrogen content. This work offers a practical method to produce nitrogen- and cobalt-rich bifunctional electrocatalysts with dodecahedral structures.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 9
·期 7
·3952-3960
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IF 11.301
Wen-Tao Wang,Nadia Batool,Tian-Heng Zhang,Jiao Liu,Xiao-Feng Han,Jing-Hua Tian,Ruizhi Yang
The oxygen reduction reaction (ORR) plays a key role in many efficient and clean energy systems, specifically in fuel cells and metal–air batteries. As a widely used commercial ORR catalyst, Pt/C has the limitations of high price and scarce reserves. Metal–nitrogen–carbon (M–N–C) is considered as one of the most promising alternatives to replace noble metal catalysts. However, how to balance the high catalytic activity and stability is still a major challenge. In this study, we report a novel non-noble metal composited catalyst, Fe–N–C@Ti3C2Tx, synthesized by a facile separated pyrolysis strategy. The Fe-doped Zeolitic Imidazolate Framework-8 (ZIF-8) was converted to Fe–N–C by carbonization firstly, which was then mixed with few-layered Ti3C2Tx and pyrolyzed together to obtain Fe–N–C@Ti3C2Tx composites. This separated pyrolysis strategy can not only ensure the high carbonization temperature required by Fe–N–C for high catalytic activity but also avoid the damage of MXene caused by high pyrolysis temperature. Thus, Fe–N–C@Ti3C2Tx exhibited excellent ORR activity and stability in alkaline solution, including a half-wave potential of 0.887 V vs. RHE, limiting diffusion current density of 6.3 mA cm−2, and even no attenuation after 10 000 cycles in 0.1 M KOH. Meanwhile, it also exhibited surprisingly good performance in acidic solution, with a half-wave potential of 0.777 V vs. RHE, limiting diffusion current density of 5.7 mA cm−2, and only 11 mV attenuation after 10 000 cycles in 0.1 M HClO4. The superior ORR performance of the synthesized Fe–N–C@Ti3C2Tx could be attributed to the strong coupling effect between Fe–N–C and MXene, the reduced intrinsic and charge transfer impedance, and the increased electrochemically active surface area. This work here provides a new strategy for the development of M–N–C based non-noble metal-based catalysts with high activity and stability, and a promising future for applications in fuel cells and metal–air batteries.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ruina Li,Xuwen Li,Qingcheng Liu,Hua Yue,Yang Meng,Yuanyuan Tian
With the continuous advancement of fuel cell technology, the exploration and development of highly efficient non - precious - metal catalysts for the oxygen reduction reaction (ORR) have emerged as a focal point of research. Fe–N–C catalysts have attracted much attention due to their excellent performance and low cost, and coupling single-atom catalysts (SACs) with atomic clusters (ACs) is an effective method to improve catalyst activity. This study used the pyrolysis method to synthesize iron atom catalysts (Fe–N–C SACs) and iron cluster coupled catalysts (Fe–N–C SACs/ACs) on ZIF-8 carbon support. It evaluated the catalyst performance through electrochemical testing. The experimental results showed that the introduction of Fe clusters improved the half-wave potential of the catalyst to 0.399 V, which represented an 8.2 % enhancement compared to the SAC catalyst and reached 87.1 % of that of the commercial Pt–C catalyst, and reduced the Tafel slope to 61.47 mV dec −1 , effectively improving the ORR activity of the catalyst. We constructed FeN 4 single atom catalyst models and FeN 4 /Fe 4 N 6 single atom cluster catalyst models using density functional theory (DFT), analyzed their electronic structures and reaction mechanisms, and revealed the mechanism of action of iron clusters. DFT calculations showed that iron clusters altered the charge distribution of FeN 4 sites, reducing the rate determining step (RDS) (OH desorption) energy to 0.5 eV, which promoted the desorption of products and the re-adsorption of reactants. As a result, the superior electrocatalytic performance of Fe–N–C SAC/AC is attributed to the synergistic effect between iron clusters and single atoms, which is influenced by the coordination environment and provides new ideas for designing efficient ORR catalysts.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Wenxuan Fan,Xiangmei Tang,Qingfeng Yi,Guang Li
Non precious metal catalysts (NMCs) are considered to have great potential for applications in oxygen reduction reaction (ORR) and water splitting reaction (OER and HER). Compared with traditional precious metal catalysts, NMCs have the characteristics of low cost, better catalytic performance, wider applicability, and better durability. This article reports a facile method for preparing layered Co-N-C catalysts by simple ball milling and pyrolysis of a mixture of graphite, ammonium carbonate, melamine and cobalt phthalocyanine. The synthesized nanoCo@bmGr and nanoCo@bmGr-EG samples exhibit excellent performance in ORR, OER and HER. For ORR in alkaline electrolyte, the nanoCo@bmGr and nanoCo@bmGr-EG present very close Tafel slopes to Pt/C catalyst. For OER under alkaline condition, the nanoCo@bmGr and nanoCo@bmGr-EG exhibit smaller Tafel slopes than IrO 2 catalyst, and at a current density of 10 mA∙cm −2 , their potential difference with IrO 2 is only 50 and 70 mV respectively. For the chronopotentiometric tests of OER at current densities of 20 and 30 mA∙cm −2 , the two samples show lower potentials than IrO 2 . In HER testing, nanoCo@bmGr and nanoCo@bmGr-EG display very similar onset potentials and Tafel slopes to Pt/C. This work provides a simple approach for preparing catalysts with good catalytic activity for ORR/OER/HER.
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
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiahao Liu,Zhaorui Zhang,Zhihang Xu,Ye Zhu,Chenshuai Han,Wei Xiong,J. Paul Attfield,Jianrong Zeng,Siqi Liu,Minghui Yang
Electrocatalytic hydrogen peroxide (H 2 O 2 ) production via the 2e − oxygen reduction reaction (ORR) offers a sustainable alternative to the energy-intensive anthraquinone process. However, achieving cost-effective, long-term stable H 2 O 2 synthesis at industrial-level current densities remains a formidable challenge. Here, we demonstrate that Ni 3 N supported on Ti 3 CN MXene (Ni 3 N/MX) undergoes surface reconstruction during electrocatalysis, forming an active NiOOH layer that optimizes *O 2 and *OOH adsorption, thereby enhancing the 2e − ORR pathway. As a result, Ni 3 N/MX achieves an exceptional H 2 O 2 yield rate of 10.7 mol·h −1 ·g −1 with a Faradaic efficiency of 92.0%. The catalyst maintains continuous operation for over 100 h at 300 mA cm −2 , demonstrating outstanding durability. Furthermore, the estimated production cost of 70 wt% H 2 O 2 is as low as $0.21 kg −1 , underscoring the economic feasibility of this approach. This work highlights metal nitride reconstruction as a powerful strategy for advancing electrosynthesis of H 2 O 2 .
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 33
·期 5
·2007525
·
IF 27.398
Jianhua Yan,Ying Wang,Yuanyuan Zhang,Shuhui Xia,Jianyong Yu,Bin Ding
Designing stable and efficient electrocatalysts for both oxygen reduction and evolution reactions (ORR/OER) at low-cost is challenging. Here, a carbon-based bifunctional catalyst of magnetic catalytic nanocages that can direct enhance the oxygen catalytic activity by simply applying a moderate (350 mT) magnetic field is reported. The catalysts, with high porosity of 90% and conductivity of 905 S m −1 , are created by in situ doping metallic cobalt nanodots (≈10 nm) into macroporous carbon nanofibers with a facile electrospinning method. An external magnetic field makes the cobalt magnetized into nanomagnets with high spin polarization, which promote the adsorption of oxygen-intermediates and electron transfer, significantly improving the catalytic efficiency. Impressively, the half wave-potential is increased by 20 mV for ORR, and the overpotential at 10 mA cm −2 is decreased by 15 mV for OER. Compared with the commercial Pt/C+IrO 2 catalysts, the magnetic catalyzed Zn–air batteries deliver 2.5-fold of capacities and exhibit much longer durability over 155 h. The findings point out a very promising strategy of using electromagnetic induction to boost oxygen catalytic activity.
研究领域:
电化学
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材料科学
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纳米催化
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能源化学
·
物理化学
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电分析化学
·
功能材料
✓ 已验证
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2022
·
IF 3.51
Chaocheng Liu,Yinghui Li,Jiedong Cui,Zhiyun Qian,Detao Liu
Here we report a simple efficient one-step strategy to fabricate Oxidation Reduction Reaction (ORR) or/and Oxygen Evolution Reaction (OER) electrocatalysts directly from agricultural cornstalks waste with hierarchical porous structures and massive active hydroxyl groups. CaCl 2 and NH 4 Cl activators were utilized to corrode the cornstalks in order to create a mesopore N-doped hybrid structure that was sufficiently stable under the high-temperature pyrolysis process, which prevented neighboring aggregates of transition metals. The synergistic effect of N, B and Fe, Co within the hierarchical biochar structures guaranteed a favorable ORR activity of 0.848 V and OER activity of 393 mV for the CaCl 2 sample, showed better stability than commercial Pt/C and IrO 2 catalysts.
研究领域:
材料科学
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电化学
·
可再生能源
·
环境科学
·
催化
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 25
·14507-14514
·
IF 12.732
Wenyan Si,Ze Yang,Xiuli Hu,Qing Lv,Xiaodong Li,Fuhua Zhao,Jianjiang He,Changshui Huang
Zero valence palladium (Pd(0)) nanoparticles have been reported to be more favorable to the oxygen reduction reaction (ORR) than palladium oxide (PdO). However, PdO is normally concomitant in Pd(0) nanoparticles. Herein, we developed an inventive method to prepare pure Pd(0) nanoparticles supported with hydrogen-substituted graphyne (Pd/HsGY) and its nitrogen-doped sample (Pd/N–HsGY). Pd(0) nanoparticles were obtained by reducing the atomically dispersed bivalent Pd, which is easy to be anchored on HsGY. The unique sp-hybridized carbon atoms in HsGY exhibited obvious extrinsic charge compensation to maintain the supported Pd nanoparticles to zero valence state. The as-prepared samples, especially Pd/N–HsGY, displayed excellent activity for ORR, higher than that of commercial Pd/C and Pt/C. In an alkaline medium, the mass activity of Pd/N–HsGY at 0.8 V (vs. RHE) was 2.1 times higher than that of Pd/C, and 1.7 times higher than that of Pt/C. While in an acidic medium, the mass activity of Pd/N–HsGY was 17.7 and 1.6 times Pd/C and Pt/C, respectively. Pd/N–HsGY based Zn–air battery exhibited higher power density than Pt/C-based battery and superior stability for more than 300 hours. Density functional theory calculations confirmed that Pd(0) nanoparticles, Pd/HsGY and Pd/N–HsGY were favorable to ORR. This method brings new perspectives for designing zero valence metal nanoparticles for electrocatalytic applications.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
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
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2020
·Vol. 45
·期 5
·7120-7128
·
IF 3.741
Menglu He,Jia Jia,Qing Sun,Weixin Zhang
SUMMARY Li-O 2 battery has attracted much attention due to its ultra-high theoretical energy density in the field of electrochemical energy storage. The introduction of efficient electrocatalyst can effectively accelerate the reaction rate of ORR and OER, so as to improve the coulomb efficiency and poor cycle stability of Li-O 2 battery. In this work, a novel hollow N-doped carbon sphere is prepared by using MOF and polystyrene as template, and act as highly efficient oxygen electrocatalyst for rechargeable Li-O 2 batteries. The hollow structure can provide enough oxygen diffusion channel, deposition and decomposition space for reduction products. N doping into the hollow carbon structure can increase the charge density of adjacent carbon atoms and enhance its catalytic activity of ORR/OER. As a result, the Li-O 2 battery using the hollow N-doped carbon sphere as air cathode exhibited an high specific capacity of 18 762 mAh/g (at a current density of 500 mA/g) and remarkable cycling stability of 212 cycles (at a current density of 500 mA/g and limited capacity of 1000 mAh/g), outperforming the carbon material with common structure. This work highlights the importance of air cathode structure and efficient catalyst, provides a new idea for the design of air cathode of Li-O 2 battery, and expands the scope of future research.
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
CARBON
·
2022
·
IF 11.307
Run Wu,Xixi Wang,Lei Ge,Zehao Zheng,Yijun Zhu,Chuan Zhou,Jinglin Yuan,Shiliang Zhu,Yuxing Gu,Wei Zhou,Zongping Shao
Zinc-air batteries (ZABs) have sparked great interest, but their wide-ranging applications are limited by sluggish cathode reactions (ORR and OER). In this work, a multifunctional 3D catalyst (FeNi alloy/porous carbon) was easily fabricated by introducing Fe 3+ and Ni 2+ to modulate in-situ vapor phase grown carbon nanotubes. The as-prepared catalyst FNSNC73-800 displays abundant mesoporous, massive structural defects , and multiple active sites, which greatly facilitate the transport of oxygen species and charge transfer during the reaction. Due to the excellent ORR and OER performance, FNSNC73-800 shows a narrow voltage gap (Δ E ) of 0.76 V, which is superior to recent reports. Notably, the secondary zinc-air battery with this catalyst displays a high-peak power density (210 mW cm −2 ), while maintaining an ultra-low potential gap (0.74 V) after a long-term charge-discharge cycle of 200 h. This effort presents a facile strategy for designing economical and efficient 3D catalysts for zinc-air batteries and more energy devices.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 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）