Journal of Physical Chemistry C
·
2021
·
IF 4.126
Shuchang Wu,Guodong Wen,Yang Su,Xiaoli Pan,Hua Yan,Jiangyong Diao,Hongyang Liu
The non-noble metal and nitrogen cofunctionalized carbon (M–N–C) attract enormous attentions in heterogeneous catalysis. However, the fabrication of the M–N–C systems commonly rely on fossil resource based carbon, while the exploitation of biomass derived materials often suffer from issues such as tedious procedures, complex composition of the biomass and excessive dosage of the dopant precursor. In this study, a direct and large-scale, bottom-up method was developed for the fabrication of the sustainable iron and nitrogen cofunctionalized carbon (FeNC) in a green and sustainable way. The obtained FeNC possessed well-defined structure as well as uniformly distributed iron species. The catalytic results suggested that FeNC could serve as efficient catalyst for the selective reduction of nitroarenes. The FeNx species played an important role, while the N-doped carbon matrix may also involve in the reaction.
研究领域:
催化
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材料科学
·
可持续化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shiyu Zuo,Yan Wang,Jinquan Wan
Peroxymonosulfate (PMS) activation technology has important application value in treating emerging contaminant (ECs), but it still faces challenges in achieving efficient electron transfer and metal valence cycling. In this study, the interfacial electric field characteristics of FeNC catalysts were adjusted by introducing N C defects to affect the electron transfer process, thereby enhancing the catalytic performance of PMS. It is found that in the Fe N C structure, the shift of the charge generates an interfacial electric field, which can promote the directional transfer of electrons. Through quantitative structure–activity relationship (QSAR) analysis, it was confirmed that the defect played a decisive role in regulating the interfacial electric field and improving the catalytic reaction efficiency. The interfacial electric field-mediated superexchange interaction realizes the electron donor effect of organic pollutants and the effective electron transfer between the Fe site, accelerates the electron cycling of the Fe site, and realizes the rapid and stable catalysis of PMS. The increase of the occupancy state distribution of d orbitals near the Fermi level provides favorable conditions for electron transitions and catalytic activation of PMS. ECs can be converted into environmentally friendly, non-toxic and harmless substances through. This defect-controlled interface electric field strategy realizes rapid electron directional transfer, which provides a new solution for improving the catalytic efficiency of PMS and the safe treatment of ECs in water.
研究领域:
环境科学
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材料科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Mengting Lu,Mingjun Xu,Jingsen Bai,Jinjing Tao,Xinying Li,Xinyi Li,Meiling Xiao,Changpeng Liu,Wei Xing
Perfluorosulfonic-acid (PFSA) ionomers are indispensable binders in FeNC cathodes for proton transport, yet their mobility during ink drying often causes non-uniform redistribution, generating locally thick ionomer layers that partially block Fe-N x sites. Here we strategically regulated the FeNC catalyst/ionomer interface by incorporating a pre-crosslinked carbon-ionomer framework, in which the ionomer is anchored to conductive carbon prior to ink formulation. This design converted the ionomer from a freely migrating phase into a pre-associated phase, thereby stabilizing its interfacial configuration during drying and mitigating the aggregation of catalyst particles. Microstructural analyses revealed improved dispersion of catalyst aggregates and a thinner, more uniform ionomer layer in the resulting composite cathode. Electrochemical analyses showed an increased electrochemically accessible interface and higher fractions of accessible Fe-N x sites, accompanied by reduced charge transfer resistance and lowered pressure-independent oxygen transport resistance, indicating primary alleviation of activation polarization. Consistent with these mechanistic gains, the optimized cathode delivered a nearly 1.39-fold increase in peak power density compared with a conventional cathode under identical cell conditions. These findings identified the regulation of the ionomer interfacial state as a key to improving site utilization in PGM-free cathodes and provided a generalizable strategy for architecting catalyst layers.
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Chanez Maouche,Yongying Wang,Chao Cheng,Wenlong Wang,Yi Li,Waqar A. Qureshi,Pengwei Huang,Ali Amjad,Yazhou Zhou,Juan Yang
Iron-nitrogen-carbon (Fe N C) catalysts derived from zeolitic-imidazolate frameworks (ZIFs) are worldwide accepted to be the most promising candidates for the oxygen reduction reaction (ORR), but the insufficient stability, the low FeN x exposure and poor density restrict their ORR activity. Here, we demonstrate a strategy to synthesize FeN x sites embedded in a micro/mesoporous N, S co-doped graphitic carbon (Fe N C/MUS) by tuning the ligand linkers via the addition of 2-undecylimidazole as a co-ligand in ZIF precursors, and optimizing the electronic structure of Fe center by an in-situ addition of thiourea molecules as sulfur (S) source. 2-undecylimidazole offered an open porous structure to incorporate more FeN x , while the S-doping increased the density of FeN x . Besides, 2-undeclyimidazole cooperatively with S-doping caused favorable changes into the catalyst structure, particularly improved the exposure and density of FeN x sites and doubled the Brunauer-Emmetter-Teller surface area to 1132 m 2 g −1 contrasted to the pristine Fe N C/M (544 m 2 g −1 ). Fe N C/MUS displayed an accelerated ORR activity with a higher half-wave potential of 0.86 V (vs. reversible hydrogen electrode (RHE)) than that of Pt/C (0.84 V) in addition of a longer durability with a 11 % of activity decay after 30 000 s in alkaline media. This work offers a new insight to design optimal ZIFs precursor and a facile electron withdrawing S-doping strategy for efficient electrocatalysis .
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
Joule
·
2024
·
IF 38.6
Jia-Ning Liu,Chang-Xin Zhao,Juan Wang,Xuan-Qi Fang,Chen-Xi Bi,Bo-Quan Li,Qiang Zhang
Refreshing the record of the electrocatalytic activity for bifunctional oxygen electrocatalysis is the first priority of developing next-generation rechargeable zinc-air batteries. A Δ E indicator to evaluate the bifunctional electrocatalytic activity has stagnated with a record of Δ E > 0.60 V for decades. Herein, a bifunctional oxygen electrocatalyst is developed to afford an ultrahigh bifunctional electrocatalytic activity of Δ E = 0.57 V and realize high-performance rechargeable zinc-air batteries. Specifically, atomically dispersed Fe-N-C sites and NiFeCe layered double hydroxides are integrated to afford a composite FeNC@LDH electrocatalyst, following the guidance of the data-driven analysis. The FeNC@LDH electrocatalyst demonstrates a record-breaking electrocatalytic activity of Δ E = 0.57 V, far exceeding the state-of-the-art level by ca. 60 mV. Practical ampere-hour-scale zinc-air batteries are constructed with a capacity of 6.4 Ah and cycle under 1.0 A and 1.0 Ah conditions. This work affords a record-breaking bifunctional electrocatalyst for ampere-hour-scale zinc-air batteries in future application scenarios.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.8
Wenxuan Lu,Simin Wang,Yuxuan Xu,Jiayi Zhong,Xiao Xia Wang,Kun Zhao,Yunfei Gao,Fuchen Wang
Intermetallic Pt with an L10-PtM structure has been considered a promising oxygen reduction reaction (ORR) catalyst for proton exchange membrane fuel cells (PEMFC) due to its reduced Pt usage and high activity. However, it suffers from issues of agglomeration during high-temperature annealing compared with its L12-Pt3M counterparts. Meanwhile, attempts to utilize the advantages of both L10-PtM and L12-Pt3M are often limited by their difficulties in material synthesis. Herein, we support intermetallic Pt particles on single-atom metal–nitrogen–carbon (M–N–C) and destabilized Fe–N sites via H2 pretreatment during the carbonization. As a result, the synthesized O-PtCo@FeNC(5H) sample displays co-presence of both L10-PtM and L12-Pt3M phases with a size distribution of 3.20 ± 0.52 nm, achieving enhanced catalytic activity and stability (mass activity (MA) = 1.23 A mgPt–1, 89.1% MA retention after 30,000 cycles). Furthermore, the membrane electrode assembly (MEA) test shows an enhanced MA of 0.471 A mgPt–1 and a peak power density of 1.288 W cm–2 in H2–air conditions. Additionally, the synthetic strategy can be extended to other M–N–C supports, including CoNC and NiNC. Overall, this work demonstrates a strategy for integrating the advantages of L10-PtM and L12-Pt3M by the use of a modified M–N–C single-atom support.
✓ 已验证
DOI
高影响因子
Small
·
2026
·
IF 11.8
Ru-Jia Chen,Zhen-Hua Zhong,Yi-Yang Lin,Zhen-Yu Sun,Hai-Kui Zou,Wei Liu,Guang-Wen Chu,Alex W. Robertson,Bao-Chang Sun,Jian-Feng Chen
The performance of FeNC single atom catalysts (SACs) is significantly influenced by the porous architecture of their N-doped carbon substrates. Although the pore structure of FeNC SACs has been widely investigated from a chemical methodology perspective, the role of synthesis process engineering has received much less attention. To address this, high-gravity technology is introduced during the precursor preparation stage to achieve intensive molecular mixing. This approach successfully yields FeNC SACs with a well-defined hierarchical micro-mesoporous structure. The resulting catalyst exhibits a narrower mesopore size distribution (4–6 nm), a higher specific surface area (800.3 m 2 ·g −1 ), and a more positive half-wave potential (0.899 V) for the oxygen reduction reaction (ORR) compared to a reference sample produced in a conventional stirred tank reactor. Density functional theory (DFT) analysis further indicates that the abundant mesopores induce carbon defects, thereby enhancing the intrinsic ORR activity. Moreover, when integrated into a zinc-air battery and an anion-exchange membrane fuel cell, the catalyst delivers high peak power densities of 259.5 and 860 mW·cm −2 , respectively, highlighting its potential for practical applications.
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产品关联
DOI
高影响因子
Materials Chemistry Frontiers
·
2024
·Vol. 8
·期 14
·2592-2598
·
IF 6
Jinfu Hou,Yongqi Jian,Chengjie Chen,Dengke Zhang,Fangyan Xie,Jian Chen,Yanshuo Jin,Nan Wang,Xiang Yu,Hui Meng
FeNC is a promising non-precious metal catalyst that can replace platinum-based catalysts in proton-exchange membrane fuel cells (PEMFCs) and zinc–air battery applications. The study utilized Fe-ZIF-8 as a precursor to improve the oxygen reduction reaction (ORR) activity of the catalyst. This was achieved by growing ruthenium particles of approximately 0.32 μm in situ using a physical milling method under a reducing gas atmosphere. This paper demonstrates that in situ grown ruthenium nanoparticles can alter the spin state of iron atoms from the high-spin state FeN4(II)-(t42ge2g) to the medium-spin state FeN4(II)-(t52ge1g). This alteration changes the interactions of the π* antibonding orbitals of the oxygen and thus improves the ORR activity. The rotating ring-disk (RDE) electrode test resulted in a half-wave potential of (E1/2) + 0.80 V vs. RHE in 0.1 M HClO4, indicating remarkable ORR performance. Zinc–air battery tests showed a high peak power density of 148 mW cm−2.
研究领域:
材料科学
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催化化学
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能源科学
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产品关联
DOI
高影响因子
Journal of Materiomics
·
2022
·
IF 8.589
Wei Lu,Shuhan Chen,Haifeng Zhang,Jiajun Qiu,Xuanyong Liu
H 2 O 2 and glutathione (GSH) are critical redox molecules in the organism. Abnormal levels of cellular H 2 O 2 and GSH are closely related to some diseases. Thus, it is imperative to detect H 2 O 2 and GSH efficiently. In this work, Fe N C single atom nanozymes (SANs) with both peroxidase and oxidase-mimicking activities were successfully prepared with the help of formamide condensation by one-step hydrothermal method. The Fe N C SANs show excellent peroxidase-like activity, which possess a higher affinity for H 2 O 2 and 3,3′,5,5′-tetramethylbenzidine (TMB) than horseradish peroxidase (HRP). Then, based on the chromogenic reaction of TMB, a colorimetric biosensor to detect H 2 O 2 and GSH was developed. This biosensor has the linear ranges of 10–600 μmol/L for H 2 O 2 with a low detection limit of 4.360 μmol/L and 100–400 μmol/L for GSH with a low detection limit of 78.33 μmol/L. Besides, this colorimetric biosensor exhibited a good recovery of H 2 O 2 and GSH in diluted human serum. Finally, the Fe N C SANs were encapsulated into agar gel to self-quantitatively detect GSH by naked eyes. This work provides a non-pyrolytic way to prepare SANs, which broadens the synthetic method of SANs and may promote the development of SANs for biosensor application.
研究领域:
生物化学
·
医学诊断
·
纳米材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Ting Yang,Nan Li,Da Wei,Chao Xie,Yahui Yang,Hao Jiang
Iron coordinated with nitrogen (FeN x ) sites hosted in the micropores of carbon substrate offer excellent performance for the oxygen reduction reaction (ORR). Achieving a highly exposed and dispersed FeN x sites accessible for ORR is still challenging to date. In this work, two-dimensional hexagonal carbon nanosheets supported FeN x moieties (FeNC-NaCl- T ) were synthesized via a molten NaCl-assisted pyrolysis strategy. Benefit from the high specific surface area (1371.635 m 3 ·g −1 ) and highly dispersed FeN x sites, the optimized FeNC-NaCl-900 exhibits superior ORR activity with a high half-wave potential of 0.90 V in alkaline electrolyte. Impressively, with FeNC-NaCl-900 as the cathode catalyst in aqueous zinc–air battery, achieving a remarkable performance with a high peak power density of 177 mW·cm −2 and competitive durability (200 h). Furthermore, the Al-air battery equipped with FeNC-NaCl-900 attained an ultrahigh specific capacity of 2257.48 mAh·g −1 at a large discharge current of 100 mA cm −2 . These findings provide guidance for the development of high performance FeNC catalysts and their applications in metal-air batteries.
研究领域:
材料科学
·
电化学
·
能源存储与转换
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Jingshun Shen,Qi Liu,Qiqi Sun,Jianwei Ren,Xue Liu,Zuoxu Xiao,Chuanwang Xing,Yuexing Zhang,Guangwu Yang,Yanli Chen
A novel two-dimensional (2D) single-atom Fe/N/C catalyst (Fe 1 Zn 30 NC PDI ) has been prepared upon pyrolyzing a well-designed quasi-Fe-/Zn-phthalocyanine-based polymer (qFePc 1 @qZnPc 30 @PDI). In the qFePc 1 @qZnPc 30 @PDI precursor, qFePc moieties containing Fe-N 4 sites are efficiently segregated by lots of qZnPc moieties connected together by perylene linkers, which not only leads to the larger specific area in the resulting Fe 1 Zn 30 NC PDI but more importantly ensures the in-situ formation of Fe-N 4 sites on the self-supporting 2D N-doped carbon backbone. Impressively, Fe 1 Zn 30 NC PDI exhibites its superior oxygen reduction reaction (ORR) electro-catalytic activity and peroxidase (POD)-like activity. For ORR in an alkaline medium, it exhibites a much higher onset potential of 0.97 V and half-wave potential of 0.89 V than 20 wt% Pt/C catalyst with good durability of 92 % retention rate after 20000 s. And, Fe 1 Zn 30 NC PDI also shows better peak power density (86 mW cm −2 ) compared with 20 wt% Pt/C in Zn-air battery. Benefiting from the specific POD-like activity of Fe-N 4 , the Fe 1 Zn 30 NC PDI also shows excellent and selective performance in colorimetric H 2 O 2 sensing, with the ultrafast response (30 s), a low limit of detection (10 nM), and good robustness. This work sheds light on a promising design concept for synthesizing 2D polymer-derived single-atom multifunctional catalysts.
研究领域:
材料科学
·
电化学
·
分析化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hao Xu,Lihui Xiao,Peixia Yang,Xiangyu Lu,Lilai Liu,Dan Wang,Jinqiu Zhang,Maozhong An
Zeolitic imidazole framework (ZIF)-derived iron–nitrogen-carbon (Fe N C) materials are expected to be high-efficiency catalysts for oxygen reduction reaction (ORR). However, increasing the density of active sites while avoiding metal accumulation still faces significant challenges. Herein, solvent environment engineering is used to synthesize the Fe N C containing dense Fe-N x moieties by adjusting the solvent during the ZIF precursor synthesis process. Compared with methanol and water/methanol, the aqueous media can provide a more moderate Fe content for the ZIF precursor, which facilitates the construction of high-density Fe-N x sites and prevent the appearance of iron-based nanoparticles during pyrolysis. Therefore, the Fe N C(C) nanocubes synthesized in an aqueous media have the highest single atom Fe loading (0.6 at%) among the prepared samples, which presents excellent oxygen reduction properties and durability under alkaline and acidic conditions. The advantage of Fe N C(C) is proven in Zn-air batteries, with outstanding performance and long-term stability.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）