TALANTA
·
2021
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IF 6.057
Xuemin Huang,Qingfeng Liu,Cuimin Wu,Zhenyu Lin,Aiwen Huang,Bin Qiu
As a popular controllable-released carrier, intelligent hydrogels are often used in drug delivery and disease therapeutics. Meanwhile, benefit from the mimic-enzyme activity performance, Fe–N–C nanozymes have been widely used in sensing and analysis. However, the combination of intelligent hydrogels with specific degradability and Fe–N–C nanozymes with enhanced activity in one system to achieve controllable and sensitive detection is rare. Herein, we combine intelligent hydrogel with mimic peroxidase activity enhanced Fe–N–C nanozymes to construct a ratiometric fluorescence probe for sensitive detection of hyaluronidase (HAase). The modification of copper ions has been proved to enhance the mimic enzyme activity of Fe–N–C nanozymes greatly. Cu 2+ modified Fe–N–C nanozymes were embedded in hyaluronic acid hydrogel. In the presence of HAase, the HA hydrogel structure was hydrolyzed and released Cu 2+ -Fe-N-C nanozymes gradually. The released Cu 2+ -Fe-N-C nanozymes are used to catalyze the hydrogen peroxide system so that o-phenylenediamine is oxidized to orange fluorescent 2, 3-diaminophenolazine (DAP). Due to the electrostatic interaction , the fluorescence resonance energy transfer can occur between the negatively charged copper nanoclusters emitted by 430 nm and the positively charged DAP emitted by 560 nm. The activity of HAase was monitored according to the ratio of fluorescence intensity at 560 nm and 430 nm (F560/F430). The linear range of this method is 0–10.0 U/ml and the detection limit is 0.43 U/mL (S/N = 3). This strategy has been further applied to biological samples successfully.
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高影响因子
Advanced Science
·
2021
·Vol. 8
·期 22
·2101824
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IF 16.806
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Fenton-like reactions with persulfates as the oxidants have attracted increasing attentions for the remediation of emerging antibiotic pollutions. However, developing effective activators with outstanding activities and long-term stabilities remains a great challenge in these reactions. Herein, a novel activator is successfully synthesized with single iron atoms anchored on porous N-doped carbon (Fe-N-PC) by a facile chemical vapor deposition (CVD) method. The single Fe atoms are coordinated with four N atoms according to the XANES, and the Fe-N 4 -PC shows enhanced activity for the activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The experiments and density functional theory (DFT) calculations reveal that the introduction of single Fe atoms will regulate the main active sites from graphite N into Fe-N 4 , thus could enhance the stability and tune the PMS activation pathway from non-radical into radical dominated process. In addition, the N atoms connected with single Fe atoms in the Fe-N 4 -C structure can be used to enhance the adsorption of organic molecules on these materials. Therefore, the Fe-N 4 -C here has dual roles for antibiotics adsorption and PMS activation. The CVD synthesized Fe-N 4 -C shows enhanced performance in persulfates based Fenton-like reactions, thus has great potential in the environmental remediation field.
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高影响因子
Frontiers in Chemistry
·
2020
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IF 3.693
Rauf Muhammad,Wang Jingwen,Iqbal Waheed,Abbas Mazhar,Khan Sayed Ali,Khan Qudrat Ullah,Ren Xiangzhong,Zhang Peixin,Li Yongliang
The exploration of noble metal-free catalysts with efficient electrochemical performance toward oxygen reduction reaction in the acid electrolyte is very important for the development of fuel cells technology. Novel pyrolyzed heteroatom-doped Fe/N/C catalysts have been regarded as the most efficient electrocatalytic materials for ORR due to their tunable electronic structure, and distinctive chemical and physical properties. Herein, nitrogen- and sulfur-doped (Fe/N/C and Fe/N/C-S) electrocatalysts were synthesized using ferric chloride hexahydrate as the Fe precursor, N-rich polymer as N precursor, and Ketjen Black EC-600 (KJ600) as the carbon supports. Among these electrocatalysts, the as prepared S and N-doped Fe/N/C-S reveals the paramount ORR activity with a positive half-wave potential value (E1/2) 0.82 at 0.80 V vs. RHE in 0.1 mol/L H2SO4 solution, which is comparable to the commercial Pt/C (Pt 20 wt%) electrocatalyst. The mass activity of the Fe/N/C-S catalyst can reach 45% (12.7 A g−1 at 0.8 V) and 70% (5.3 A g−1 at 0.95 V) of the Pt/C electrocatalyst in acidic and alkaline solutions. As result, ORR activity of PGM-free electrocatalysts measured by the rotating-ring disk electrode method increases in the following order: Fe/N/C
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Guolong Lu,Xin Men,Ruoqi Tang,Zhida Wang,Hao Cui,Tongxi Zheng,Mi Wang,Haoqi Yang,Zhenning Liu
Transition metal and nitrogen co-doped carbon electrocatalysts are promising candidates to replace the precious metal platinum (Pt) in oxygen reduction reactions (ORR). Unfortunately, the electrochemical performance of existing electrocatalysts is restricted due to limited accessibility of active sites. Inspired by jellyfish tentacles, we design an efficient ORR micro-reactor called Fe-N x /HC@NWs. It features abundant exposed Fe-N x active sites dispersed on nitrogen-doped cubic carbon cages, which have a hierarchically porous and hairy structure. The accessible, atomically dispersed Fe-N x sites and the elaborate substrate architecture synergize to provide the catalyst withremarkable ORR catalytic activity, extraordinary long-term stability, and favorable methanol tolerance in an alkaline electrolyte ; overall, its performance is comparable to that of commercial carbon-supported Pt. Our synthesis is facile and controllable, paving a new avenue toward advanced non-precious metal-based electrocatalysts for energy storage and conversion .
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Bin Hu,Yongqing Yang,Wei Cao,Xixi Wang,Chuan Zhou,Yiyang Mao,Lei Ge,Ran Ran,Wei Zhou
The high cost and unfavorable catalytic performance for oxygen reduction reaction (ORR) is one of the crucial obstacles that impede widely commercialization of proton-exchange membrane fuel cells (PEMFCs). Herein, we provide a novel, mass-producible ORR catalyst made of low-loading (10 wt%) Pt nanoparticles bound to patchy nitrogen-doped carbon (PNC) with uniformly dispersed FeN 4 sites (Pt/FeN 4 -PNC). The derived catalyst exhibits significantly improved catalytic activity and stability, obtaining a promising mass activity (MA) of 0.94 A mg pt −1 at 0.9 V (vs. RHE) with a negligible decay after 30,000 cycles accelerated durability test (ADT). In the fuel-cell assessment (under H 2 -Air conditions at 80 ℃), the Pt/FeN 4 -PNC and Pt/FeN 4 -PNC-10 g (scaled-up production) achieved peak power densities of 1.13 W cm −2 and 1.14 W cm −2 , respectively, and retained 88.5 % and 88.1 % of the initial values after 30,000 voltage cycles (0.60–0.95 V). The patchy structure of PNC substrate guarantees fast electron routes and resistance to corrosion. With the FeN 4 active sites in the PNC substrate, the oxygen molecules are concurrently reduced on the surfaces of the carbon substrate and Pt nanoparticles, thereby causing the ORR reaction zone on the catalyst layer to expand.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xing Li,Lei Xing,Chunyu Zhang,Shudan He,Fanghua Liu,Zhen Chen,Huazhen Chang,Junhua Li
Catalytic solvent regeneration is widely considered a promising solution for addressing the intensive heat duty of amine-based carbon dioxide (CO 2 ) capture. This highly challenging application has motivated researchers to develop excellent catalysts with high activity and durability. In this study, we engineered active and durable Fe − N − C catalyst coated with high-graphitization carbon layers (labeled Phen − Fe − N − C) through a secondary thermal pyrolysis treatment. The multiple graphite layers and atomic metal sties were verified by experimental characterization and coordination structure analysis. The improved graphite layers further enhanced the activity of Fe − N − C sites, providing more acid sites for proton-electron transfer and C − N breaking during solvent regeneration (or CO 2 desorption). Thus, the maximal CO 2 desorption rate increased by 50 % when Fe − N − C was used compared with that of the blank case, and the rate further increased by 27 % when Phen − Fe − N − C was used. After 15 days of hydrothermal testing, the single Fe atom over the spent catalysts presented no significant aggregation or dissolution in the solvent, validating the durability of Phen − Fe − N − C. This work demonstrates a feasible and novel strategy to improve M − N − C materials for efficient and robust CO 2 desorption from amine solvents toward energy-saving CO 2 capture.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Siyuan Sun,Fan Yang,Xiaoyun Zhang,Jinxiu Qian,Kexin Wei,Junpu An,Yang Sun,Shuyang Wang,Xi Li,Yongfeng Li
Transition metal single-atom catalysts (SACs) have been widely used in oxygen reduction reactions (ORR) and oxygen evolution reaction (OER) due to its greatest atomic utilization and low costs, which catalytic performance can be further enhanced by electron distribution adjustment. Herein, we synthesized a carbon-encapsulated FeS/Fe 3 C nanoparticles doped carbon-based Fe single atom catalyst from fluid catalytic cracking (FCC) slurry though a one-pot pyrolysis. The synergistic effect between FeS/Fe 3 C nanoparticles and Fe single atom structure (FeN x ) promotes the ORR/OER processes, which may due to the reduction of the adsorption free energy of intermediates. Meanwhile, the polyaromatic hydrocarbon in FCC slurry enhances the graphitization of catalyst to facilitate charge transfer in electrocatalysis process, and the carbon-encapsulated nanoparticles sites possess higher stability and dispersion. As a result, the optimized catalyst (FeS/Fe 3 C@Fe-N-C) presents a high nanoparticles dispersion and graphitization level, which has a higher ORR catalytic ability (E 1/2 = 0.91 V vs RHE) compared with commercial Pt/C (20 wt%, E 1/2 = 0.879 V vs RHE) and a similar OER catalytic ability (E 10 = 0.1.506 V vs RHE) compared with RuO 2 (E 10 = 1.518 V vs RHE). A liquid Zn-air battery assembled with FeS/Fe 3 C@Fe-N-C show a peak power density of 113 mW cm −2 and an open potential of 1.432 V. This work sheds light on a new method to design transition metal active sites carbon based single-atom catalyst for enhanced ORR and OER processes.
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Small
·
2024
·
IF 13
Ziyi Xu,Shihao Wang,Wenmao Tu,Ling Shen,Lu Wu,Shilong Xu,Haining Zhang,Hongfei Pan,Xiao-Yu Yang
Stable, efficient, and economical bifunctional electrocatalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are needed for rechargeable Zn–air batteries. In this study, a directional electron transfer pathway is exploited in a spatial heterojunction of Co y Ni x @Fe─N─C heterogeneous catalyst for effective bifunctional electrolysis (OER/ORR). Thereinto, the Co/Ni alloy is strongly coupled to the Fe─N─C support through Co/Ni─N bonds. DFT calculations and experimental findings confirm that Co/Ni─N bonds play a bridging role in the directional electron transfer from Co/Ni alloy to the Fe─N─C support, increasing the content of pyridinic nitrogen in the ORR-active support. In addition, the discovered directional electron transfer mechanism enhances both the ORR/OER activity and the durability of the catalyst. The Co 0.66 Ni 0.34 @Fe─N─C with the optimal Ni/Co ratio exhibits satisfying bifunctional electrocatalytic performance, requiring an ORR half-wave potential of 0.90 V and an OER overpotential of 317 mV at 10 mA cm −2 in alkaline electrolytes. The assembled rechargeable zinc–air batteries (ZABs) incorporating Co 0.66 Ni 0.34 @Fe─N─C cathode exhibits a charge–discharge voltage gap comparable to the Pt/C||IrO 2 assembly and high robustness for over 60 h at 20 mA cm −2 .
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高影响因子
APPLIED ENERGY
·
2025
·
IF 11
Xianda Sun,Baibin Ma,Jinxu Hao,Zirui Wu,Yi Li,Hao Liu,Yuandong Yang,Xiaohan Ren
The ammonia crossover that poisons the conventional cathode catalysts and damages the cell performance and efficiency is one of the paramount bottlenecks limiting the development of direct ammonia fuel cells (DAFCs). Synthetizing the ammonia tolerance catalysts has been proven to be an effective avenue to solve the above-mentioned problems, however, the mass and charge transports within the anti-ammonia poisoning electrodes has not been fully elucidated. Herein, an alkaline DAFC with anti-ammonia poisoning Fe-N-C cathode is reported, and the main effort is expended on investigating the impact of mass and charge transports on cell performance, internal resistance, and operating stability. The alkaline DAFC exhibits a thermodynamic efficiency as high as 88.6 %, higher than that of hydrogen-based fuel cells. The preliminary experimental results indicate that the performance of DAFC with anti-ammonia poisoning Fe-N-C cathode is higher than that of conventional Pt/C cathode under the same catalyst loading. The impressive open-circuit voltage of 0.74 V and peak power density of 107 mW cm −2 are obtained under atmospheric pressure and 80 °C, which is primarily ascribed to both the anti-ammonia poisoning of Fe-N-C catalyst and the facilitated mass and charge transports. Furthermore, the voltage curve of DAFC is quite stable during the constant-current discharging at 100 mA cm −2 for 10-h, demonstrating the good durability of DAFC with anti-ammonia poisoning Fe-N-C cathode.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xu Lin,Danyang Li,Shiqing Huang,Panpan Sun,Yan Huang,Shitao Wang,Lirong Zheng,Dapeng Cao
The limited activity of atomically-dispersed M-N-C electrocatalysts severely restricts their applicability in the oxygen reduction reaction (ORR) for proton exchange membrane fuel cells (PEMFC). Herein, we design and synthesize Se-doped Fe-N-C hierarchical porous electrocatalyst (FeN 4 /SeC 2 ) by optimizing carbon structure and FeN 4 coordination environment. The FeN 4 /SeC 2 electrocatalyst exhibits outstanding ORR activity in 0.1 mol L –1 HClO 4 , and the resulting PEMFC presents a peak power density of 1.20 W cm –2 in H 2 -O 2 condition at a back pressure of 200 kPa, ranking in the top levels among most reported non-precious metal catalyst-based fuel cells. The lower O 2 transfer resistance of FeN 4 /SeC 2 -based membrane electrode assembly than FeN 4 -based one means faster O 2 transport in triple-phase boundary (TPB), and Density functional theory calculation further reveals that the synergistic catalysis between porous SeC 2 and FeN 4 -OH species can efficiently lower the energy barriers for the rate-determining step of the ORR. In short, the outstanding performance of FeN 4 /SeC 2 in PEMFC is ascribed to the Se-doping, which introduces more defects and larger mesoporosity and therefore facilitates ionomer infiltration and O 2 transfer and charge transfer in TPB. The effective strategy of enhancing mass and charge transfers in TPB is anticipated to be applicable in the construction of highly efficient ORR electrocatalysts.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Qingtao Liu,Weihao Liu,Xin Wan,Weiwei Chen,Xiaozhi Liu,Xiaofang Liu,Jiaxiang Shang,Jungang Miao,Dong Su,Xin Sun,Jianglan Shui
Zeolitic imidazolate framework-8 (ZIF-8) is widely used as precursor for carbon-supported single-metal-atom catalysts (M–N–C), but typically yields amorphous carbon with poor stability in proton-exchange-membrane fuel cells (PEMFCs). Traditional methods would lose active site density while increasing the graphitization degree. Here, this study reports that ultra-small nano ZIF-8 can produce graphene-nanostacks-based Fe–N–C that has improvements on both activity and stability. First, anti-sintering nanoporous ZIF-8 (nano-ZIF8) particles are synthesized with unit size of 8 nm (the smallest so far) using a destruction-reconstruction strategy. In situ microscopy reveals that the volatilization of Zn has a decisive effect on the graphitization degree of ZIF-8 and such process is size-dependent. Nano-ZIF8 particles have completed Zn volatilization before graphitization process beginning, leading to graphene nanostacks. These nanostacks preferentially host edge-type FeN 4 sites, which have doubled intrinsic activity and much improved stability compared with conventional Fe−N−C. In PEMFC, the catalyst achieves an activity of 48.5 mA cm − 2 @0.9V iR -free , meeting the US Department of Energy 2025 activity target. In addition, quantitative analysis of active site density is conducted in PEMFC for the first time using nitrite stripping voltammetry. The unique graphitization behavior of nano-ZIF8 paves a new avenue for advancing M–N–C catalysts.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Lin Li,Shuiyun Shen,Guanghua Wei,Xiaolin Li,Kun Yang,Qi Feng,Junliang Zhang
There remain great challenges in exploring cost-effective and highly efficient non-noble metal electrocatalysts to catalyze the oxygen reduction reaction (ORR) of proton exchange membrane fuel cells (PEMFCs). Also, a further validation on their performances under a fuel cell operating condition draws sustained attention. Herein, we report a comprehensive investigation on the ORR performances of a series of pyrolyzed Fe–N–C composites that use phenanthrolene as the nitrogen precursor, and the effects of carbon supports, transition metal precursors, and annealing temperatures are examined in detail. Electrochemical measurements combined with different physicochemical characterizations are employed to clarify the function of critical structures including the specific surface area, microstructure, nitrogen content, nitrogen type, and corresponding proportion on their ORR and fuel cell performances. It demonstrates a half-wave potential of 0.79 V and almost a four-electron pathway. When using the as-optimized Fe–N–C composite as the cathode catalyst of a PEMFC, the maximum power density reaches as high as 540 mW cm–2.
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