Carbon Letters
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2024
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IF 5.5
Long Qing,Wu Qianqi,Wen Zhiming,Wang Wei,Li Chen,Tang Huichuan,Wang Haitao,Huang Junlin,Chen Liang,Li Gangyong,Xu Wenyuan
Considering the intrinsic activity of non-precious metal oxygen reduction reaction (ORR) catalysts is typically lower than that of precious metal catalysts, it is crucial to focus on the rational design of their micro-morphology and active site. This paper employed a simple molten salt-mediated template method to fabricate a Fe 3 C composite N-doped C catalyst with a layered porous framework (Fe 3 C@NC). Tannic acid was utilized to form a strong coordination with iron to limit the grain size of Fe 3 C nanocrystals generated by high-temperature pyrolysis. Moreover, urea achieved nitrogen doping in tannic acid-derived porous carbon, while the graphite phase nitrogen-doped carbon (g-C 3 N 4 ) formed by its pyrolysis, together with the molten salt-mediated environment, jointly controlled the two-dimensional sheet-like structure of the material. The optimized Fe 3 C@NC-800 demonstrated efficient ORR performance, with an ORR half-wave potential of 0.883 V. Its application as a cathode catalyst in a liquid zinc-air battery (ZABs) exhibits a maximum power density of 211.5 mW cm −2 , surpassing that of a Pt/C-based ZAB and indicating the potential practical utility of this material.
研究领域:
材料科学
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能源化学
·
电催化
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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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.
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Catalysts
·
2026
·Vol. 16
·期 5
·462
·
IF 4.5
Danyang Zhu,Baolong Liu,Yiping Mo,Qiao Zhang,Yuhan Ma,Wenqi Dai,Wangyang Lu
Effective regulation of the adsorption strength of oxygen reduction reaction (ORR) intermediates on active sites is the key to enhancing their catalytic performance. This study proposes an axial coordination modulation strategy by successfully anchoring the dioxin-linked FePcF16-based covalent organic frameworks (COFs) onto amino-functionalized multi-walled carbon nanotubes (NH2-MWCNTs), constructing a FePcF16-COF/NH2-MWCNT hybrid catalyst. Experimental results demonstrate that the catalyst exhibits outstanding ORR activity (E1/2= 0.901 V; JL= 5.133 mA cm−2), outperforming commercial 20% Pt/C and most reported Fe-based non-precious metal catalysts. Furthermore, the robust dioxin-linked COF skeleton endows the catalyst with excellent electrochemical stability. A zinc–air battery using this catalyst as the cathode also demonstrates superior power density and cycling performance. This work provides a new strategy for designing highly efficient ORR catalysts through axial coordination environment engineering.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
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IF 8.4
Yu Qiao,Huajing Zhou,Lingxiang Zhao,Liang He,Rongrong Miao,Zilian Liu,Qingqing Guan
Chlorophenol pollutants are listed as global priority control substances due to their strong carcinogenicity and difficult biodegradability. The advanced oxidation technology based on •OH has strong oxidizability superior to other oxygen-active substances, and has become a favorable candidate for the treatment of organic pollutants in the environmental field. Among them, electrocatalytic two-electron ORR is widely used in water environment treatment as a typical electrochemical advanced oxidation (EAOP) technology. Under normal conditions, molecular oxygen (O 2 ) can be selectively reduced to hydrogen peroxide (H 2 O 2 ) by ORR two-electron reaction, and then further forms efficient hydroxyl radicals (•OH), which is used to target various refractory micropollutants.However, the electro-Fenton (EF) process faces challenges such as slow O 2 adsorption and activation, slow O−O bond cleavage, and slow ORR kinetics on the cathode due to the dissolution of metal ions. In the ORR reaction, the terminal adsorption of ∗OOH intermediates on the active site is difficult to achieve independent regulation, resulting in a slow kinetic process of directional conversion from hydrogen peroxide to hydroxyl radicals.Therefore, the removal efficiency of organic pollutants in EF process is seriously restricted by the above factors.This thesis proposes a kinetic optimization strategy based on the synergistic effect of heteronuclear bimetallic catalysts and the polarization of surface hydroxyl groups (−OH). By constructing a cobalt-iron layered double hydroxide (CoFe-LDHs) catalyst, we significantly enhance the selective generation of hydroxyl radicals along the oxygen reduction reaction (ORR) pathway, achieving efficient degradation of refractory organic pollutants such as 4-chlorophenol (4-CP). Our research reveals that CoFe-LDHs form a Fe−O−Co bridging structure through electron transfer between Fe 3+ and Co 2+ , which induces asymmetric adsorption of the O−O bond and lowers the kinetic energy barrier for O−O coupling (forming MxO−HOOH intermediates). This enables the directed conversion of •OH at low overpotentials. Therefore, the kinetic optimization strategy for catalysts based on modulating the adsorption of intermediates at active sites is not only of significant importance in current research but also provides new ideas and directions for future catalyst design and development.In particular, it shows broad application prospects in the fields of energy conversion and storage, environmental pollution control and so on.
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PubMed
高影响因子
Nanoscale
·
2024
·Vol. 16
·期 10
·5433-5440
·
IF 5.8
Lijing Yang,Junhong Ma,Yuemei Liu,Chaoyun Ma,Xue Yu,Zhaohui Chen
The development of economical and efficient platinum-based catalysts for the oxygen reduction reaction (ORR) is considered the most promising strategy for the widespread application of clean energy conversion devices. Herein, Co nanoparticles encapsulated in N-doped carbon carriers, CoCN(CDs-X), were constructed by pyrolyzing carbon dots (CDs) doped ZIF-67 and further used to anchor Pt to prepare low Pt loading catalysts, PtCoCN(CDs-X). The introduction of CDs not only improves the conductivity for efficient electron transfer, but also regulates the interaction between Pt and the CoCN(CDs-X) support and alleviates the oxidation of Pt. The optimized PtCoCN(CDs-0.10) displays decent ORR behavior with onset and half-wave potentials of 0.95 V and 0.83 V, respectively, in alkaline media and superior catalytic stability and methanol tolerance. While employing PtCoCN(CDs-0.10) as a cathode catalyst for an as-assembled zinc–air battery (ZAB), it delivers an excellent power density of 194.2 mW cm−2 and exceptional operation stability, which is indicated by a voltage efficiency loss of only 7.7% after a long cycle life of 100 h, demonstrating its great potential applications.
研究领域:
材料科学
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能源化学
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Guijun Li,Yibo Tang,Tiantian Fu,Yang Xiang,Zhongping Xiong,Yujun Si,Chaozhong Guo,Zhiqiang Jiang
The development of efficient and cost-effective bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for the commercialization of rechargeable metal-air batteries. Herein, the pyrolysis of a precursor containing g-C 3 N 4 , thiourea, cobalt chloride and ferric chloride was used to fabricate S, N co-doped carbon nanotubes functionalized with Co 3 Fe 7 alloy nanoparticles (CoFe/S-N-C). The obtained CoFe/S-N-C catalyst exhibited an ORR half wave potential of 0.855 V ( vs . RHE) in 0.1 M KOH, outperforming a commercial Pt/C catalyst ( E 1/2 = 0.844 V). The catalyst also demonstrated superior OER catalytic activity (1.588 V at 10 mA cm −2 ) relative to RuO 2 in 0.1 M KOH, thus displaying outstanding bifunctional ORR and OER activity. A rechargeable Zn-air battery fabricated using CoFe/S-N-C shows good very performance (maximum power density of 120 mW cm −2 with a specific capacity of 814 mAh g −1 ) which was superior to a Zn-air battery fabricated using Pt/C and RuO 2 as ORR and OER catalysts (92 mW cm −2 and 787 mAh g −1 , respectively). Further, the fabricated battery using CoFe/S-N-C showed good stability, offering a discharge voltage ∼ 1.10 V and a recharge voltage ∼ 2.15 V at 10 mA cm −2 over 300 cycles, evidence of the durability of the CoFe/S-N-C catalyst.
研究领域:
材料科学
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电化学
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能源存储与转换
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高影响因子
CHINESE CHEMICAL LETTERS
·
2023
·
IF 9.1
Fengxian Zhang,Xupo Liu,Ye Chen,Miao Tian,Tianfang Yang,Jing Zhang,Shuyan Gao
Fe-N X /C electrocatalysts have aroused extensive interest in accelerating sluggish oxygen reduction reaction (ORR) kinetics as potential alternatives to platinum catalysts in rechargeable Zn-air batteries (ZABs). However, the low density and poor accessibility of Fe-N X sites have severely restricted the electrocatalytic performance of Fe-N X /C. Herein, Fe, N co-doped ordered mesoporous carbon fiber bundles are prepared through a ligand-assisted strategy with nitrogen-rich 1,10-phenanthroline as space isolation agent. 1,10-Phenanthroline reveals a six-membered heterocyclic structure containing abundant nitrogen species to tightly coordinate with Fe ions , which is conducive to achieving high-density Fe-N X sites. Meanwhile, the adoption of SBA-15 as hard-templates enables the catalysts with highly ordered channels and large specific surface areas, improving the accessibility of Fe-N X sites. The optimal catalyst (PDA-Fe-900) demonstrates a positive half-wave potential of 0.84 V ( vs. RHE) in alkaline solution, outperforming the commercial Pt/C (0.83 V). In addition, PDA-Fe-900 delivers comparable ORR performance to commercial Pt/C in acidic electrolyte. Impressively, when PDA-Fe-900 is employed as an air cathode, it achieves large power densities of 163.0 mW/cm 2 in liquid-state ZAB and 116.6 mW/cm 2 in the flexible solid-state ZAB. This work provides an efficient ligand-assisted pathway for fabricating catalysts with dense and accessible Fe-N X sites as high-performance ORR electrocatalysts for ZABs.
研究领域:
材料科学
·
电化学
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高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Jiaxiang Chen,Lei Qiu,Zheling Li,Guanhui Gao,Wenhua Zhong,Peixin Zhang,Yongji Gong,Libo Deng
Oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are the rate-controlling and/or energy-intensive reactions of numerous energy conversion and storage devices. It is a great challenge to attain a high catalytic efficiency with a single electrocatalyst towards these reactions simultaneously. Herein, a porous carbon was prepared by pyrolysis of chitin with the assistance of CoCl 2 and ZnCl 2 and a subsequent sulfurization process, which resulted in uniform loading of Co, N and S elements. The porous and modified carbon exhibited high catalytic performance towards ORR, OER and HER. Furthermore, the catalyst was used as air electrode to construct Zn-air batteries, which showed a power of 142 mW cm −2 and discharging and charging voltages of 1.3 V and 1.74 V at 1 mA cm −2 after 100 cycles, respectively. When used as both the anode and cathode for water splitting, the voltage to achieve a 10 mA cm −2 electrolysis current was 1.58 V which was stable over 75 h of operation. The performance enhancement is attributed to the etching effect which generates defects in both carbonaceous matrix and the Co 9 S 8 crystallites during the sulfurization , as well as the doping of S and N elements which creates multiple active sites.
研究领域:
材料科学
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电化学
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能源存储与转换
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高影响因子
Nano Energy
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2015
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IF 10.325
Tao Yang,Yanxia Ma,Qingli Huang,Guojian Cao
Exploiting nanomaterials with high electrocatalytic activity toward oxygen reduction reaction (ORR) and desirable durability in acid media has been recently one of the most significant tasks for developing electrochemical devices . Pd based nanostructures have received considerable interest owing to their Pt analogous surface and ever increasing catalytic performance. We herein report a series of Pd–Ir bimetallic nanoparticles with wire or dendritic shapes in a wide composition range, which were synthesized through a facile hydrothermal strategy. Such nanostructures featured with large electrochemical active surface area (EASA), show comparable catalytic activities to that of commercial Pt catalyst. More importantly, the catalysts display much high durability, as an example, Pd 1 Ir 2 losses 6% in EASA and 12% in mass activity after 10,000 potential sweeps, in contrast to respective losses of 42% and 58% for commercial Pt/C counterparts. The remarkable durability was also revealed in actual fuel cells supplied with hydrogen and air. The work demonstrates that these Pd–Ir nanostructures with enhanced performance are promising for practical electrocatalytic applications.
研究领域:
材料科学
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电化学
·
纳米技术
·
催化
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Feng Zhang,Dongqing Zhang,Wenqi Liu,Jiyuan Miao,Xiaojin Li
Developing a feasible method to massively fabricate low-cost and efficient oxygen reduction reaction (ORR) catalysts is highly anticipated to the commercialization of fuel cells. In this work, N atoms were doped into inert sp2 configuration to alter the spin and charge distribution in the carbon matrix. The Pt/H2–N–C catalyst was successfully prepared by embedding ultralow Pt nanoparticles on N-based carbon. Results indicated that the protonated N-groups at edge sites efficiently regulated the absorption of the PtCl62– anion and widely limited the migration of Pt species at 1000 °C. The acquired Pt/H2–N–C electrocatalyst exhibited high ORR performance in the acidic electrolyte. The high-temperature proton exchange membrane fuel cell (HT-PEMFC) measurement illustrated that the open-circuit voltage and power density of the Pt/H2–N–C catalyst were higher than those of the commercial 20% Pt/C at 150 °C. This work provided a facile strategy to obtain efficient and low-cost Pt catalysts for ORR and HT-PEMFCs.
研究领域:
材料科学
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化学工程
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能源技术
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高影响因子
ChemCatChem
·
2026
·Vol. 18
·期 15
·e70976
·
IF 4.1
Yuxuan Qiao,Yan Lv,Nannan Zhao,Xueyan Wu,Rui Xue,Jixi Guo
The development of efficient and durable non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) is critical to advancing electrochemical energy devices. Herein, we report a porous, carbazole-based N-doped carbon framework catalyst embedded with Fe 2 O 3 nanoparticles and Fe-N x sites. The catalyst was synthesized via pyrolysis of N-rich hypercrosslinked polymers (NHCP), which were derived from the Friedel-Crafts reaction, followed by incorporation of hemin (Fe 2 O 3 /NHCP-2). The introduction of hemin not only preserved the pristine porous architecture but also facilitated the formation of Fe 2 O 3 nanoparticles and Fe-N x sites, and their synergistic effect enhanced the ORR kinetics in alkaline media. The optimized Fe 2 O 3 /NHCP-2 catalyst exhibited a high half-wave potential of 0.87 V and demonstrated robust long-term durability in a 0.1 M KOH solution. When employed as the cathode material in zinc-air batteries (ZABs), it delivered a peak power density of 186.84 mW cm −2 and a specific capacity of 731.37 mAh g Zn −1 . This study presents a promising non-precious metal ORR electrocatalyst for future renewable energy applications. Graphical A porous carbazole-based N-doped carbon framework embedded with Fe 2 O 3 nanoparticles and Fe-N x sites was synthesized by pyrolyzing N-rich hypercrosslinked polymers from a Friedel-Crafts reaction, then hemin incorporation. As a Zn-air battery cathode, Fe 2 O 3 /NHCP-2 delivers a power density of 186.84 mW cm −2 , high specific capacity (731.37 mAh g Zn −1 ) and OCV (1.52 V). The porous structure ensures rapid O 2 transport. Fe 2 O 3 nanoparticles and dispersed Fe-N x sites synergistically enhance ORR. This work demonstrates N-rich hypercrosslinked polymers as effective carbon precursors for high-performance ORR catalysts.
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高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.5
Xiaoyang Dong,Jinxing Wang,Jingdong Yang,Wen Zeng,Guangsheng Huang,Jingfeng Wang
Magnesium (Mg)–air batteries are regarded as promising large-scale energy-storage devices because of their high theoretical energy density, low material cost, intrinsic safety, and environmental benignity. Nevertheless, their practical deployment is severely hindered by sluggish oxygen reduction reaction (ORR) kinetics at the cathode. Herein, nanoscale transition-metal–nitrogen-doped carbon (M-N-C, M = Fe, Co, Ni) electrocatalysts─denoted FNC, CNC, and NNC─are prepared by argon-pyrolysis of Prussian blue analogues (PBAs). The cationic and anionic ligands are systematically varied to tailor the crystal phase, pore architecture, and nanoscale M-Nx coordination environment. Comprehensive characterization shows that CNC possesses the highest density of well-dispersed Co-Nx active nanosites embedded in a graphitic matrix. This ensures rapid electron transfer and abundant accessible active centers. Electrochemical tests in alkaline (0.1 M KOH) and neutral (3.5 wt % NaCl) electrolytes demonstrate that CNC delivers the most robust ORR activity and stability (CNC > FNC > NNC) via a near-ideal 4 e pathway. Meanwhile, CNC exhibits better stability than commercial Pt/C in both alkaline and neutral electrolytes. As the cathode nanocatalyst in Mg-air batteries, CNC is found to yield a peak power density of 19.14 mW/cm2─only 0.66 mW/cm2 below that of commercial Pt/C. The decisive role of nanoscale M-Nx coordination environments in boosting ORR kinetics is thus elucidated. This work provides a nanomaterials-driven strategy for developing high-performance, cost-effective electrocatalysts for Mg-air batteries.
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