DALTON TRANSACTIONS
·
2016
·Vol. 46
·期 6
·1803-1810
·
IF 4.177
Ganesan Anandhababu,Syed Comail Abbas,Jiangquan Lv,Kui Ding,Qin Liu,Dickson D. Babu,Yiyin Huang,Jiafang Xie,Maoxiang Wu,Yaobing Wang
Progress in the development of efficient electrocatalysts for oxygen reduction reactions is imperative for various energy systems such as metal–air batteries and fuel cells. In this paper, an innovative porous two-dimensional (2D) poly-iron–phthalocyanine (PFe–Pc) based oxygen reduction electrocatalyst created with a simple solid-state chemical reaction without pyrolysis is reported. In this strategy, silicon dioxide nanoparticles play a pivotal role in preserving the Fe–N4 structure during the polymerization process and thereby assist in the development of a porous structure. The new polymerized phthalocyanine electrocatalyst with tuned porous structure, improved specific surface area and more exposed catalytic active sites via the 2D structure shows an excellent performance towards an oxygen reduction reaction in alkaline media. The onset potential (E = 1.033 V) and limiting current density (I = 5.58 mA cm−2) are much better than those obtained with the commercial 20% platinum/carbon electrocatalyst (1.046 V and 4.89 mA cm−2) and also show better stability and tolerance to methanol crossover. For practical applications, a zinc–air (Zn–air) battery and methanol fuel cell equipped with the PFe–Pc electrocatalyst as an air cathode reveal a high open circuit voltage and maximum power output (1.0 V and 23.6 mW cm−2 for a methanol fuel cell, and 1.6 V and 192 mW cm−2 for the liquid Zn–air battery). In addition, using the PFe–Pc electrocatalyst as an air cathode in a flexible cable-type Zn–air battery exhibits excellent performance with an open-circuit voltage of 1.409 V. This novel porous 2D PFe–Pc has been designed logically using a new, simple strategy with ultrahigh electrochemical performances in Zn–air batteries and methanol fuel cell applications.
研究领域:
电化学
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能源材料
·
催化化学
·
纳米材料
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金属-空气电池
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燃料电池
·
功能高分子材料
✓ 已验证
DOI
高影响因子
Carbon Energy
·
2025
·
IF 24.2
Fangyan Liu,Mengye Wang,Jiawen Liu,Feng Gao,Jiahui Lin,Jiaqing He,Feng Zhu,Chuan Liu,Zhang Lin
Lead (Pb)–zinc (Zn) slags contain large amounts of Pb, causing irreversible damage to the environment. Therefore, developing an effective strategy to extract Pb from Pb–Zn slags and convert them into a renewable high-value catalyst not only solves the energy crisis but also reduces environmental pollution. Herein, we present a viable strategy to recycle Pb and iron (Fe) from Pb–Zn slags for the fabrication of efficient methylammonium lead tri-iodide (r-MAPbI 3 ) piezocatalysts with single-atom Fe–N 4 sites. Intriguingly, atomically dispersed Fe sites from Pb–Zn slags, which coordinated with N in the neighboring four CH 3 NH 3 to form the FeN 4 configuration, were detected in the as-obtained r-MAPbI 3 by synchrotron X-ray absorption spectroscopy. The introduction of Fe single atoms amplified the polarization of MAPbI 3 and upshifted the d-band center of MAPbI 3 . This not only enhanced the piezoelectric response of MAPbI 3 but also promoted the proton transfer during the hydrogen evolution process. Due to the decoration of Fe single atoms, r-MAPbI 3 showed a pronounced H 2 yield of 322.4 μmol g −1 h −1 , which was 2.52 times that of MAPbI 3 synthesized using commercially available reagents. This simple yet robust strategy to manufacture MAPbI 3 piezocatalysts paves a novel way to the large-scale and value-added consumption of Pb-containing waste residues.
研究领域:
材料科学
·
环境科学
·
催化
·
能量转换
·
无机化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 35
·18147-18155
·
IF 14.511
Jin Li,Kaicai Fan,Hongliang Jiang,Fenghong Lu,Lixiu Cui,Bin Li,Qi Zhang,Gao-Chao Fan,Lingbo Zong,Lei Wang
Fe–N–C single atom electrocatalysts (SAECs) with porphyrin-like Fe–N4 species are one of the most promising alternatives to the platinum-group-metal-based electrocatalysts used for oxygen reduction reaction (ORR). However, limited attention is paid on delicately optimizing the free energy barrier of Fe–N4 active sites through heteroatom doping in the carbon skeleton. Herein, Fe single atoms (SAs) on heteroatoms N- and P-codoped porous honeycomb-like carbon (Fe–N4/NP-PHC) have been rationally designed. The as-developed Fe–N4/NP-PHC catalyst with abundant accessible active sites showed an impressive onset potential (Eonset = 1.0 V) and half-wave potential (E1/2 = 0.89 V) under low electrocatalyst loading capacity, which is more positive than those of Pt/C and most SAECs. Encouragingly, the experimental results and DFT calculations systematically demonstrated that the optimized adsorption energy of the Fe–N4 sites in the P-doped carbon matrix facilitated the release of OH* and thus boosted the ORR performance. The metal–air battery containing Fe–N4/NP-PHC exhibited high peak power density and long-term working feasibility with a low voltage gap at large current densities. This study demonstrates that P doping in carbon matrix is an effective strategy to promote catalytic properties and presents a novel avenue for developing high-performance electrocatalysts for various electrochemical reactions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Mengxue Yang,Ruixian Wu,Shengshuai Cao,Yanwei Li,Sisi Huo,Wei Wang,Zhen Hu,Xing Xu
Herein, we prepared two kinds of single-atom catalysts (SACs) with uniformed coordination structures (M−N 4 , M = Fe, and Cu) for evaluating the versatile pathways of peroxymonosulfate (PMS) activation by different metal sites. Fe-SAC exhibited a higher catalytic performance than that of Cu-SAC for chloroquine phosphate (CQP) oxidation. Results showed that the high-valent iron-oxo species accounted for 74.5 % for CQP oxidation in Fe-SAC/PMS system, while radicals (SO 4 •– and HO • ) dominated the CQP oxidation (58.3 %) in Cu-SAC/PMS system, which was associated to the different spin-state of the metal sites for PMS adsorption and breakage of O O in PMS as well as the intermediates in versatile pathways. The SACs were then fixed onto the catalytic filter for PMS activation , which showed stable and effective catalytic performance for versatile recalcitrant organics. Overall, this work not only provided the atomic-level knowledge on PMS activation, but also gave the potential applications of Fenton-like for water remediation.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Environmental Science & Engineering
·
2025
·Vol. 19
·期 12
·1-17
·
IF 6.4
Wei Biao,Liu Daoqing,Peng Ran,Zhou Yi,Li Qianwei,Zhao Huazhang
The remediation of nitroaromatic-contaminated water systems remains a critical environmental challenge, creating the urgent need for cost-effective, non-precious metal catalysts to increase wastewater biodegradability. In this study, we present an Fe/N-functionalized three-dimensional porous carbon (Fe–N–C) catalyst synthesized via a straightforward pyrolysis approach that enables efficient nitrobenzene (NB) degradation via electrochemical and chemical reduction pathways. The high-temperature pyrolysis process facilitates the iron-catalyzed reconstruction of the carbon matrix, resulting in a hierarchically porous structure with increased graphitization and uniformly distributed macrocyclic Fe–N 4 coordination sites. These structural features give the Fe–N–C catalyst exceptional electron transfer kinetics, catalytic activity, and pH adaptability, surpassing conventional graphite (GR) and nitrogen-doped carbons (NPCs) in NB reduction. Systematic evaluation of the electrochemical reduction performance revealed that the Fe–N–C electrode achieved the highest NB removal efficiency. To further assess the versatility of the catalyst, a functionalized Fe–N–C/zero-valent iron (ZVI) composite was engineered by integrating Fe–N–C as a catalytic layer onto the reductant ZVI. Compared with ZVI alone, this composite markedly increased the NB reduction efficiency. These findings provide valuable insights into the electrochemical reduction process of Fe–N–C and new directions for the rational design of efficient nitrobenzene reduction systems.
研究领域:
环境科学
·
材料科学
·
电化学
·
催化
·
水处理
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Xiaojie Tan,Fengliang Cao,Xuan Han,Libo Wang,Zhengqiu He,Jinqiang Zhang,Yikun Zhao,Wei Deng,Hui Ning,Zhongtao Li,Qingshan Zhao,Mingbo Wu
Iron-nitrogen-carbon (Fe-N-C) single-atom materials have emerged as the most promising catalysts for the oxygen reduction reaction (ORR), which yet suffers from inadequate stability arising from the attack of ·OH and HO 2 · radicals generated by H 2 O 2 . In this study, density functional theory (DFT) calculations reveal that the presence of peripheral S atoms can regulate the electronic structure of the Fe center and suppress the formation of H 2 O 2 to enhance the catalyst's durability. Thereafter, atomic Fe-N 4 with peripheral S doping is intricately engineered in defect-rich porous carbon nanoshells (Fe-NS-C) through an adsorption-pyrolysis method. The incorporation of S not only optimizes the coordination microenvironment of Fe-N 4 but also induces a larger specific surface area and richer defects. The Fe-NS-C catalyst displays remarkable ORR performance, featuring a half-wave potential (E 1/2 ) of 0.90 V. Its low H 2 O 2 yield (below 1.1 %) and excellent stability (10 mV day in E 1/2 after 10,000 cycles) further underscore the superiority of Fe-NS-C. When employed as the cathode for Zn-air battery, Fe-NS-C achieves an impressive peak power density of 230.1 mW cm −2 and stable charge/discharge potentials over an extended duration of 150 h. This study presents an effective strategy for engineering efficient and durable single-atom electrocatalysts for ORR and Zn-air batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yuan Qin,Zihao Ou,Chaozhong Guo,Yao Liu,Rong Jin,Chuanlan Xu,Haifeng Chen,Yujun Si,Honglin Li
Regulating the electronic structure by phosphor-doping is a preferred strategy to boost the performance of carbon-based catalysts for oxygen reduction reaction (ORR). Here, a porous Fe, P, N-codoped carbon catalyst (PCF-FeTz-900) is designed by a phytic acid-assisted thermal etching strategy, in which P atoms are first doped into the carbon matrix to form a stable P C bond, and then FeN 4 sites are produced from Fe-2,4,6-Tris(2-pyridyl)-s-triazine complex (Fe-TPTz). Theoretical calculations suggest that the electrons are transferred from the doped P atom to the neighboring FeN 4 sites, which facilitates the ORR at the Fe sites by reducing the energy barrier and the adsorption energy of intermediates. Additionally, the P-doped FeN 4 (FeN 4 P) structure manifests a lower free energy difference than that of FeN 4 and the d -band center of Fe is also lowered, which further ensures its higher ORR catalytic ability. As a result, the PCF-FeTz-900 catalyst exhibits superior ORR activity and stability in alkaline electrolyte, and the assembled primary zinc-air battery shows greater performances compared to the commercial Pt/C catalyst. This work can provide an effective pathway for modulating the performance of doped-carbon materials in energy conversion devices.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Nano Materials Science
·
2026
·
IF 20.5
Weicheng Tang,Xiaoyu Guo,Yuting Chen,Zhenyu Xiao,Yunmei Du,Jun Xing,Zexing Wu,Lei Wang,Kang Liu
The catalytic performance of single-atom catalysts primarily depends on their coordination environment. To date, research on the catalytic regulation of SACs has predominantly concentrated on the first and second coordination structures of the central atom. In this study, we demonstrate that regulating the nitrogen-mediated non-coordinated microenvironment beyond the second coordination sphere of SACs is also crucial for optimizing catalytic performance. A dual metal-organic framework precursor, ZIF-L@ZIF-8/Fc, was constructed using the “MOF@MOF” strategy, wherein ferrocene was in situ anchored within the cages of ZIF-L@ZIF-8. Notably, a ligand exchange strategy was adopted, where the 1,2,4-triazole-3,5-diamine ligand underwent ligand exchange with the dimethylimidazole ligand in the ZIF-L@ZIF-8/Fc precursor, and the e-Fe SA /CSNC catalyst rich in Fe-N 4 active sites was formed through pyrolysis. Density functional theory confirmed that the ligand exchange strategy optimized the non-coordinated microenvironment of the Fe-N 4 active sites. Consequently, the e-Fe SA /CSNC catalyst exhibits excellent performance across the entire pH range, with half-wave potentials of 0.95 V, 0.81 V, and 0.83 V in alkaline, acidic, and neutral media, respectively. Furthermore, the e-Fe SA /CSNC-based zinc-air battery and quasi-solid-state zinc-air battery show long-term cycling stability, during which the intrinsic morphology of ZIF-L is maintained, exhibiting excellent overall performance.
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Liang Dong,Jianbing Zang,Weiping Wang,Xin Liu,Yan Zhang,Jing Su,Yanhui Wang,Xiumei Han,Jinsheng Li
The metal (Fe/Co), nitrogen co-doped carbon represent an important class of oxygen reduction reaction (ORR), which can be obtained via the thermal treatment of transition-metal macrocycles (TMMs). However, the N 4 -chelate complex with metal atom (M-N 4 ) moieties as major activity site for ORR are easily destroyed to form inorganic metal species during simple pyrolysis of TMMs. In this report, polyacrylonitrile (PAN) nanofibers were prepared by electrospinning containing a small amount of hemin (chloroprotoporphyrin IX iron(III), TMMs). The electrospun nanofibers were converted into Fe, N co-doped carbon nanofibers (Fe- N -CNFs) through preoxidized and thermal treatment. The PAN macromolecules can prevent hemin from aggregation during the process of pyrolysis. The Fe elemental mapping demonstrated that Fe species probably existed in a single atom state. The Fe K-edge X-ray absorption fine structure spectrum of Fe- N -CNFs proved that the Fe-N 4 moieties have been successfully reserved. The X-ray photoelectron spectra of Fe- N -CNFs indicated that the amount of Fe-N 4 moieties increased with the increased percent of hemin. Therefore, the Fe- N -CNFs exhibited the higher catalytic activity for ORR compared with Pt electrocatalysts . Furthermore, the Fe1- N -CNFs displayed higher stability and methanol tolerance than Pt/C.
研究领域:
材料科学
·
电化学
·
纳米技术
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jingjing Li,Wei Xia,Yanna Guo,Ruijuan Qi,Xingtao Xu,Dong Jiang,Tao Wang,Yoshiyuki Sugahara,Jianping He,Yusuke Yamauchi
Iron-based single-atom catalysts (Fe-SACs) containing Fe–N 4 active sites have shown immense potential in the oxygen reduction reaction (ORR). However, the limited ability to adsorb O 2 and catalyze subsequent O–O bond breaking on Fe–N 4 sites has hindered their full potential, especially in acidic electrolytes. Here, we present an approach by utilizing a tunable curved surface to enhance the activity of Fe–N 4 active sites, with theoretical calculations, demonstrating that Fe–N 4 sites anchored on low–curvature surfaces (lc-Fe-N 4 ) is favirable for ORR. Experimental results show that the catalyst exhibits excellent catalytic activity and stability for ORR in acidic electrolytes, with a half-wave potential of 0.82 V vs. RHE, approaching that of commercial Pt/C. This work develops an approach for promoting the catalytic activity by anchoring atomically dispersed Fe–N 4 sites, unlocking their potential for extended use in electrocatalytic and energy storage applications.
研究领域:
材料科学
·
电化学
·
催化
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
·
2025
·
IF 8.9
Ying Li,Zelin Wu,Xiaoyu Liu,Bingkun Huang,Jing Zhang,Yanbiao Shi,Chuan-Shu He,Zhaokun Xiong,Xingxing An,Bo Lai
Extensive research has been devoted to single-atom activation of persulfates in recent years. However, mechanistic understanding of the distinct interactions between different persulfates ( i.e. , peroxymonosulfate (PMS) and peroxydisulfate (PDS)) and the coordination environments of single-atom catalysts (SACs) remains critical for advancing their practical applications. Herein, we developed a Fe-N 4 SAC exhibiting dual activation capabilities for both PMS and PDS. Intriguingly, experimental results revealed divergent activation mechanisms: PMS activation was predominantly mediated via single-site reactions generating singlet oxygen ( 1 O 2 ), whereas PDS activation proceeded through both dual-site and single-site pathways involving concurrent 1 O 2 generation and electron transfer processes. Density functional theory calculations further demonstrated that the geometric alignment between the inter-site distances of Fe-N 4 centers and the molecular dimensions of PDS serves as the key determinant for enabling the electron transfer pathway. This fundamental structure-reactivity correlation suggests that the intrinsic molecular-scale differences between PMS and PDS govern their distinct interaction mechanisms with Fe-N 4 SACs. Finally, the scale-up experiments realized nearly complete sulfamethoxazole degradation during 120 h continuous operation without obvious decline in both the Fe-N 4 /PMS and Fe-N 4 /PDS systems. This work provides fundamental insights into molecular-scale effects on persulfate activation mechanisms, establishing new design principles for SACs optimization in advanced oxidation processes.
研究领域:
催化
·
环境化学
·
材料科学
·
物理化学
·
水处理技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xin Li,Wanrong Bu,Ke Zhu,Yuwen Chen,Xiaoying Liang,Bin Wang,Yuchen Wang,Kai Yan
Single-atom catalysts (SACs) as photo-Fenton-like catalysts have attracted widespread attention in water purification. However, the development of SACs with renewability, cleanliness, high mass loading, and raw material abundance is a formidable challenge to achieve efficient pollutant removal. In this study, we fabricated high-performance Fe-nanocluster embedded biomass-derived carbon (Fe/Bio-C) from Ficus altissima wastes for quinolone antibiotics degradation. The high-angle annular dark-field scanning transmission electron microscopy with aberration correction (AC-HAADF-STEM) and X-ray absorption fine structure spectroscopy (XAFS) revealed that the Fe/Bio-C exhibited a porous structure with abundant Fe-N 4 active sites. The Fe/Bio-C catalysts achieved an exceptional efficiency of 98.6 % for the removal of the representative quinolone antibiotic, namely lomefloxacin (LOM), within 30 min. Furthermore, an in-depth exploration was conducted to assess the influence of reaction parameters on degradation performance, kinetics, toxicity, and mechanism. The free radical quenching experiments and electron paramagnetic resonance (EPR) spectra demonstrated the existence of ·O 2 − , 1 O 2 , ·OH, SO 4 · − in the reaction system and the ·O 2 − radicals played a relatively important role in the degradation progress. This work broaden the avenue for constructing metal-nanocluster photocatalysts with the high reactivity, low metal leaching, and universality to various pollutants.
研究领域:
环境科学
·
材料科学
·
化学工程
·
水处理
✓ 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）