CARBON
·
2025
·
IF 11.6
Sabarinathan Ravichandran,Angappan Kausalya,Xinru Ji,Senthilkumar Lakshmipathi,Huaneng Su,Daifen Chen,Jie Yu
Defect engineering coupled with heteroatom-induced electronic modulation is crucial for developing highly active metal-free carbon electrocatalysts for anion exchange membrane fuel cells (AEMFCs). However, precisely identifying active configurations in dual-heteroatom-doped carbon and controlling the ORR pathway remains challenging. Herein, we present a lignin-based supermolecule-regulated pyrolysis strategy for synthesizing N, O co-doped porous carbon (LNOC) with a large surface area of 549.7 m 2 g −1 and a hierarchical porous structure. The optimized LNOC-900 catalyst demonstrates excellent ORR activity, featuring a half-wave potential (E 1/2 ) of 0.86 V vs. RHE and a high kinetic current density (j k ) of 83.29 mA cm −2 at 0.85 V, surpassing the benchmark commercial Pt/C electrocatalyst. When employed as the cathode in AEMFCs, LNOC-900 achieves a maximum peak power density (1.05 W cm −2 ) and current density (3.30 A cm −2 ) at 0.8 V. Density functional theory (DFT) reveals that N/O co-doping and defect engineering synergistically optimize ORR intermediate adsorption, with pyridinic-N embedded in a defective sp 2 carbon matrix, facilitating O–O bond cleavage via charge density modulation at defect sites. This work presents a sustainable, low-cost path to next-generation energy storage and conversion devices.
研究领域:
材料科学
·
电化学
·
能量转换与存储
·
可持续能源
·
碳材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 12
·5829-5837
·
IF 8.867
Yuanyuan Dong,Yijie Deng,Jianhuang Zeng,Huiyu Song,Shijun Liao
We report a composite catalyst in which binary transition metal nitride nanoparticles (NPs) were mounted on nitrogen-doped reduced graphene oxide (TiCoNx/N-rGO). The catalyst exhibited outstanding oxygen reduction activity in an alkaline medium. In its optimal form, our catalyst yielded a half-wave potential of 0.902 V (vs. RHE), ∼30 mV more positive than that of the commercial Pt/C catalyst, and its current density at 0.9 V (vs. RHE) reached 2.51 mA cm−2. The ORR activity of our transition metal nitride-mounted N-rGO was much higher than the activities of transition metal nitride alone or N-rGO alone, revealing a strong synergistic effect between the two materials. Further, the catalyst mounted with Ti and Co binary NPs exhibited higher ORR activity than the catalyst mounted solely with Ti nitride NPs, indicating the significant improvement gained by the addition of cobalt. XPS analysis results showed that the mounting of transition metal nitride clearly changed the amount and distribution of N species in the catalyst, causing the percentage of active pyridinic-N species to increase significantly. Moreover, changes in the binding energies of C and Ti atoms proved the synergy between TiCoNx NPs and N-rGO. We therefore ascribe the superior electrochemical activity of our TiCoNx/N-rGO catalyst to this synergy and to the improvement resulting from the addition of Co. In addition to its outstanding ORR activity, this catalyst also showed excellent stability and methanol tolerance, making it a promising Pt-free ORR catalyst for alkaline H2/O2 fuel cells and direct methanol fuel cells.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Lei Cao,Xinghai Zhou,Zhenhuan Li,Kunmei Su,Bowen Cheng
Nitrogen and fluorine co-doped hierarchical honeycomb-like carbon nanofibers (N F-CNFs-950) are prepared by electro-blown spinning technology and high temperature calcination . It possesses large specific surface area, micro/meso/macro hierarchical through-pore structure, high pyridine-N and graphite-N content. These characteristics make it exhibit an outstanding alkaline electrocatalytic oxygen reduction reaction (ORR) activity (half wave potential of 0.833 V vs reversible hydrogen electrode and current density of 5.48 mA cm −2 ). In particular, the introduction of the ionic C F/N F successfully avoids the inactivation of pyridine N in the carbon skeleton due to protonation in the acidic electrolyte. And the ionic C F/N F activated pyridine N work synergistically with graphite N to promote N F-CNFs-950 to exhibit an acidic ORR activity (half wave potential of 0.606 V vs reversible hydrogen electrode and current density of 5.58 mA cm −2 ) that is only second to commercial Pt/C. Importantly, the N F-CNFs-950 catalyst exhibits much better methanol tolerance and electrochemical stability in both alkaline and acidic environments.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Lin Gong,Xiaodong Li,Qi Zhang,Bing Huang,Qiang Yang,Guangcheng Yang,Yousong Liu
Transition metal quantum dots (QDs) are ideal electrocatalysts due to their short ion diffusion path, high atom utilization and effective electron transfer properties. However, a lack of facile and large-scale synthesis strategy limits their industrial production and commercial application. In this study, a triaminoguanidine salt-induced one-step deflagration method is first reported for the ultrafast (hundreds of milliseconds) and gram-scale synthesis of Co 3 O 4 QDs-C 3 N 4 /rGO as an efficient oxygen reduction reaction (ORR) catalyst with high durability. The deflagration reaction process is carefully studied and the formation mechanism is proposed to explain the controllable synthesis of Co 3 O 4 QDs. An optimized sample is capable of achieving an excellent ORR performance in terms of an onset potential of 0.97 V (vs. RHE, equivalent to Pt/C) and the limited current density of −5.33 mA·cm −2 at 0.35 V (vs. RHE, ~7% higher than that of Pt/C). It is believed that this simple and effective synthesis strategy will open up an exciting new avenue to the future design and facile synthesis of Co 3 O 4 or other QDs-based functional materials.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
YuXin Zhao,Jiaxian Liu,Tong Zhang,FangXun Liu,Man Zheng,Kun Shi,JinPeng Liu,Yufan Zhang,Huan Wang
The exploration of an inexpensive catalyst with effective oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) activities to replace precious metal electrocatalysts has been of great interest in recent years. In this paper, CNT@Co-Fe/FePc composites were synthesized with high efficiency using a self-assembly strategy. In the synthesis process, carbon nanotubes (CNTs) were synthesized as the base material using crab shells as templates and honey as the carbon and nitrogen source. CoFe alloy nanoparticles derived from CoFe-based prussian blue analogs were self-assembled and anchored on CNTs, and then iron phthalocyanine with Fe-N 4 portion was coupled with CNTs by π-π stacking. Finally formed a homogeneous and stable composite material. The self-assembly method is simple and efficient to achieve good metal loading. The prepared CNT@Co 2 -Fe 1 /FePc exhibits excellent catalytic performance and stability for OER and ORR in alkaline electrolyte . The overpotential at 10 mA cm −2 of CNT@Co 2 -Fe 1 /FePc for OER is 343 mV with a very small Tafel slope of 43.59 mV dec −1 . CNT@Co 2 -Fe 1 /FePc has high methanol tolerance and persistence for ORR. This work provides a strategy for the construction of transition metal-carbon composite electrocatalytic materials with excellent catalytic performance and stability for OER and ORR reactions.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 46
·17447-17459
·
IF 8.307
Wenhao Tang,Jialin He,Kewei Teng,Lei Gao,Ruiyu Qi,Yirui Deng,Ruiping Liu,Ang Li,Huadong Fu,Chang-an Wang
3d Transition-metal nitrogen–carbon nanocomposites (T–N–C, T = Fe, Co, Ni, etc.) with highly active M–Nx sites have received much attention in the field of rechargeable zinc–air battery research. However, how to rationally dope metallic elements to decorate T–N–C catalysts and enhance their electrocatalytic performances remains unclear. Herein, we demonstrated that cobalt-doped Fe-rich catalysts are effective in improving ORR performances by density functional theory (DFT) calculations. On this basis, we reported a kind of novel bifunctional electrocatalyst of hollow nitrogen-doped carbon tubes with coexisting M–N–C single atoms and alloy nanoparticles (denoted FexCoyNiz@hNCTs). Benefiting from the synergistic effect between different components, the as-prepared Fe4Co1Ni2@hNCT catalyst exhibited a small overpotential difference of 0.75 V between an OER potential at 10 mA cm−2 and an ORR half-wave potential, as well as an excellent zinc–air battery performance, when serving as the air cathode. This work provided a scalable design concept for multi-metal doping toward high-performance T–N–C electrocatalysts.
研究领域:
电化学
·
材料科学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
Advanced Composites and Hybrid Materials
·
2025
·Vol. 8
·期 4
·1-12
·
IF 21.8
Wang Lijuan,Shi Yaqin,Wang Yuan,Jia Chunijang,Hou Jie,Su Yizhen,Xu Ben Bin,Liao Zhijian,Zhu Linhua
Synergistic effect between M-N X sites and M X O Y particles in hierarchical porous M–N-C catalysts holds great promises in boosting oxygen reduction reaction (ORR). In this work, 1,4-dicyanobenzene was utilized as a molecular template to prepare the hierarchical porous Fe–N-C catalysts with size-tunable Fe 3 O 4 particles for enhanced ORR in Zn-air battery. The as-prepared Fe 3 O 4 #Fe–N/C DB0.1 owned a half-potential of 0.90 V vs RHE, exceeding that of commercial 20%Pt/C (E 1/2 = 0.82 V vs RHE), showing a maximum power density of 321 mW cm −2 in a homemade Zn-air battery. Density functional theory (DFT) calculations indicate that the electronic interaction between Fe 3 O 4 and Fe-N 4 sites enhances the adsorption energy of *OOH, effectively optimizing the energy barrier for *O formation, significantly reducing the limiting energy barrier. Such superior ORR activity in Fe 3 O 4 #Fe–N/C originated from the optimized hierarchical pores and synergistic effect between Fe-N X sites and Fe 3 O 4 particles. This work provides a new and facile template strategy for engineering hierarchical porous carbon-based materials to achieve highly efficient catalytic reactions.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
·
能量存储与转换
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 13
·17094-17104
·
IF 2.478
Zou Jizhao,Peng Minggui,Liu Peng,Zhang Shengjiao,Zhang Qi,Deng Fei,Zeng Xierong,Li Xiaohua
It is of great allure to construct nitrogen-doped hierarchical porous carbon to replace Pt-based catalysts for efficient ORR. Here, nitrogen-doped hierarchical porous carbon (NHPC) was prepared by carbonizing ZTIF-1 and KOH activating. The resultant NHPC4-700 catalyst exhibits a hierarchical porous structure and high specific area (2404 m 2 g −1 ), which promoted the exposure of enough active sites as well as simultaneously enhanced the electron transfer rate, shorten the mass transfer pathway, enhanced ionic conductivity and carbon wetting. The results are capable of remarkably improving the ORR activities of carbon materials. The NHPC4-700 catalyst exhibits a great catalytic performance with onset potential at 0.90 V and limiting current density of − 6.0 mA cm −2 , which is close to commercial Pt/C electrocatalyst. Meanwhile, the NHPC4-700 catalysts had better stability and methanol resistance than that of Pt/C toward ORR. These superior electrochemical properties of the NHPC4-700 catalysts were closely related to their nitrogen-doped hierarchical porous structure and high specific area.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
RUSSIAN JOURNAL OF GENERAL CHEMISTRY
·
2025
·Vol. 95
·期 6
·1455-1463
·
IF 0.8
Chen X.,Xiu X.,Zhuang X.,Sun H.,Dong C.
Developing cost-effective and efficient non-precious metal oxygen reduction catalysts (ORRs) is crucial for advancing renewable energy technologies. This study reports the synthesis and characterization of a novel non-precious metal catalyst, N–C–Fe-600, synthesized via a simple two-step method. Pyrolysis of NH 2 –MIL-88(Fe) under an inert atmosphere, followed by acidic treatment, yielded a porous N–C–Fe-600 material featuring a high surface area and a substantial concentration of active Fe–N x sites. Electrochemical characterization revealed that N–C–Fe-600 exhibits ORR activity comparable to commercial Pt/C catalysts, along with significantly enhanced stability and methanol tolerance. The catalyst demonstrates a near-ideal four-electron transfer pathway, suggesting its potential as a viable alternative to platinum-based catalysts in fuel cells.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
·
能源技术
✓ 已验证
DOI
高影响因子
Energy & Environmental Science
·
2016
·Vol. 9
·期 12
·3736-3745
·
IF 25.427
Haihua Wu,Haobo Li,Xinfei Zhao,Qingfei Liu,Jing Wang,Jianping Xiao,Songhai Xie,Rui Si,Fan Yang,Shu Miao,Xiaoguang Guo,Guoxiong Wang,Xinhe Bao
A coordinatively unsaturated copper–nitrogen architecture in copper metalloenzymes is essential for its capability to catalyze the oxygen reduction reaction (ORR). However, the stabilization of analogous active sites in realistic catalysts remains a key challenge. Herein, we report a facile route to synthesize highly doped and exposed copper(I)–nitrogen (Cu(I)–N) active sites within graphene (Cu–N©C) by pyrolysis of coordinatively saturated copper phthalocyanine, which is inert for the ORR, together with dicyandiamide. Cu(I)–N is identified as the active site for catalyzing the ORR by combining physicochemical and electrochemical studies, as well as density function theory calculations. The graphene matrix could stabilize the high density of Cu(I)–N active sites with a copper loading higher than 8.5 wt%, while acting as the electron-conducting path. The ORR activity increases with the specific surface area of the Cu–N©C catalysts due to more exposed Cu(I)–N active sites. The optimum Cu–N©C catalyst demonstrates a high ORR activity and stability, as well as an excellent performance and stability in zinc–air batteries with ultralow catalyst loading.
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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jun Liu,Zhou Peng Li,Bin Hong Liu
We report our facile and efficient approach for synthesizing Co-Fe alloy based oxygen reduction reaction (ORR) catalysts, in which alloy nanoparticles are encapsulated in nitrogen-doped carbon nanostructures . The catalysts with high hierarchical porosities are fabricated at an appropriate temperature of 775 °C without a further acid leaching treatment after pyrolysis due to the use of ZnO nanoparticles as auto-removable templates. Co/Fe atomic ratio is found to greatly influence the ORR catalytic activity. The catalyst with Co/Fe = 1 exhibits the best catalytic performance by showing an ORR onset potential of 0.99 V and a half-wave potential of 0.87 V (vs. RHE) in 0.1 M KOH, as well as 0.98 V and 0.83 V (vs. RHE) in 0.5 M H 2 SO 4 , better than or approaching the performance presented by a commercial 28.6 wt% Pt/C catalyst. The Zn-air battery using the synthesized CoFe@N-C catalyst delivers a higher power density at ambient conditions by air-breathing than the one using the 28.6 wt% Pt/C catalyst. Relatively higher atomic concentrations of both Fe and Co as well as more graphitic nitrogen in the surface of CoFe@N-C detected by X-ray photoelectron spectroscopy (XPS) may account for its excellent ORR catalytic activities both in alkaline and acidic environments.
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
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2026
·
IF 4.6
Yu Wang,Danyang Wu,Jiao wu,Xizhen Zhang,Yongze Cao,Baojiu Chen
We breakthrough the conventional high-temperature paradigm for synthesizing transition metal catalysts by discovering 500 °C as a critical metastable window in ultrafast (>1500 °C/s) Joule heating synthesis. This kinetically confined thermal shock at precisely 500 °C uniquely terminates metal aggregation while locking abundant pyridinic-N sites (2.86 at.%) that effectively anchor highly dispersed Fe and Co species, simultaneously sculpting a defect-rich carbon matrix. This unique combination, inaccessible in traditional pyrolysis, unlocks exceptional synergistic activity. Consequently, the 500 °C-engineered NC-FeCo catalyst achieves an oxygen reduction record: half-wave potential (0.92 V) surpassing Pt/C (0.85 V) and 1500 °C-treated analogs (0.85 V), while delivering near-theoretical 4e − selectivity (<1.2% H₂O₂), negligible decay (ΔE = 3 mV/5000 cycles), and superior methanol tolerance. Our work establishes sub-second 500 °C thermal shock as an innovative platform for metastable dual-metal electrocatalysis.
✓ 已验证
产品关联
DOI
高影响因子