A Cu and Fe dual-atom nanozyme mimicking cytochrome c oxidase to boost the oxygen reduction reaction

Du, Cuicui; Gao, Yijing; Chen, Hengquan; Li, Ping; Zhu, Shuyun; Wang, Jianguo; He, Qinggang; Chen, Wei

doi:10.1039/d0ta06485h

Cited by 142 publications

(116 citation statements)

References 48 publications

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“…A dominant EXAFS FT peak founded in the related fitting curves of Cu SAs/CN around 1.44 Å can be ascribed as the Cu—N scattering path. [ 30 , 32 , 33 ] Whereas no Cu—Cu coordination peak at 2.2 Å can be observed, suggesting that Cu exists as an isolated atom that is atomically dispersed on the CN matrix. [ 29 ] Meanwhile, the EXAFS fitting curves perfectly reproduced the experimental EXAFS FT experimental curves of Cu SAs/CN (Figure 1f and Figure S8 , Supporting Information), Cu foil and CuO (Figure S9 , Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

Atomically Dispersed Cu Nanozyme with Intensive Ascorbate Peroxidase Mimic Activity Capable of Alleviating ROS‐Mediated Oxidation Damage

et al. 2021

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Ascorbate peroxidase (APX) as a crucial antioxidant enzyme has drawn attentions for its utilization in preventing cellsfrom oxidative stress responses by efficiently scavenging H 2 O 2 in plants. For eliminating the specific inactivation of natural APXs and regulating the catalytic activity, single-atom nanozymes are considered as promising classes of alternatives with similar active sites and maximal atomic utilization efficiency to natural APXs. Herein, graphitic carbon nitride (g-C 3 N 4 ) anchored with isolated single copper atoms (Cu SAs/CN) is designed as an efficient nanozyme with intrinsic APX mimetic behavior. The engineered Cu SAs/CN exhibits comparable specific activity and kinetics to the natural APXs. Based on the density functional theory (DFT), Cu-N 4 moieties in the active center of Cu SAs/CN are determined to exert such favorable APX catalytic performance, in which the electron transfer between Cu and coordinated N atoms facilitates the activation and cleavage of the adsorbed H 2 O 2 molecules and results in fast kinetics. The constructed Cu SAs/CN nanozyme with superior APX-like performance and high biocompatibility can be applied for effectively protecting the H 2 O 2 -treated cells against oxidative injury in vitro. These findings report the single-atom nanozymes as a successful paradigm for guiding nanozymes to implement APX mimetic performance for reactive oxygen species-related biotherapeutic.

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Section: Resultsmentioning

confidence: 99%

Atomically Dispersed Cu Nanozyme with Intensive Ascorbate Peroxidase Mimic Activity Capable of Alleviating ROS‐Mediated Oxidation Damage

et al. 2021

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“…It is observed that the binding energy of M‐N x in Cu/Fe−NC exhibits a negative shift of 0.12 eV and positive shift of 0.15 eV as compared with Fe−N−C and Cu−N−C, respectively, which indicates Cu species donor electrons to N x ‐Fe configuration and Fe species withdraw electrons from Cu‐N x sites. Profiting from above electronic mobility of Cu→Fe, local electron transfer may have occured, which further attract intermediates of ORR [14d,25] . In addition, the Cu/Fe−NC possesses the highest fraction of C−N according to C 1s deconvolution (17.05 %, Figure S6) and the highest total fraction of active N dopants (62 % from pyridinic‐N, M−N and graphitic‐N) among the four materials (Figure 3d and Table S3), which is attributed to the modulation of micro‐meso porous structure to be beneficial for N coordination and configuration [18b,26] …”

Section: Resultsmentioning

confidence: 98%

Fe‐ZIF8 Coating Cu Foil Derived Carbon as A pH‐Universal Electrocatalyst for Efficient Oxygen Reduction Reaction

Yang

Xie

Tang

et al. 2021

Chemistry A European J

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It is a great challenge to fabricate highly efficient pH‐universal electrocatalysts for oxygen reduction reaction (ORR). Herein, a facile strategy, which includes coating the Fe modified ZIF8 on Cu foil and in situ pyrolysis to evaporate and dope Cu into the MOF derived carbon, is developed to fabricate Fe/Cu−N co‐doped carbon material (Cu/Fe−NC). Profiting from the modulated electron distribution and textual properties, well‐designed Cu/Fe−NC exhibits superior half‐wave potential (E1/2) of 0.923 V in alkaline, 0.757 V in neutral and comparable 0.801 V in acid electrolytes, respectively. Furthermore, the ultralow peroxides yield of ORR demonstrates the high selectivity of Cu/Fe−NC in full pH scale electrolytes. As expected, the self‐made alkaline and neutral zinc‐air batteries equipped with Cu/Fe−NC cathode display excellent discharge voltages, outstanding peak power densities and remarkable stability. This work opens a new way to fabricate highly efficient and pH‐universal electrocatalysts for ORR through strategy of Fe/Cu−N co‐doping, Cu foil evaporation and carbon defects capture.

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“…Nevertheless, Pt‐based catalysts also have severely hampered the development of AABs, which is caused by the high cost, limited resources, Pt dissolution, and carbon corrosion in strong alkaline medium. [ 9,10 ] To address these issues, it is urgent to explore and develop efficient and durable nonprecious metal ORR electrocatalysts to substitute Pt usage.…”

Section: Introductionmentioning

confidence: 99%

Electronic Structure Regulation of Iron Phthalocyanine Induced by Anchoring on Heteroatom‐Doping Carbon Sphere for Efficient Oxygen Reduction Reaction and Al–Air Battery

Luo

Chen

Xue

et al. 2021

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Aluminum–air batteries (AABs) are deemed as a potential clean energy storage device. However, exploiting high‐efficiency and stable oxygen reduction reaction (ORR) electrocatalysts in AABs is still a challenge. Iron phthalocyanine (FePc) shows a great prospect in ORR but still far from Pt‐based catalysts. Here, the hybrid electrocatalysts of monolayer FePc and hollow N,S‐doped carbon spheres (HNSCs) are innovatively constructed through π–π stacking to achieve high dispersion. The resulting FePc@HNSC catalyst exhibits an outstanding ORR activity, outperforming that of pristine FePc and even most Fe‐based catalysts reported to date. Moreover, the AAB using FePc@HNSC catalyst not only demonstrates a superior power density than the battery with Pt/C, but also displays stable discharge voltages and excellent durability. Furthermore, the theoretical calculations confirm that the charge distribution and d‐band center of the Fe atom in FePc are efficiently optimized by hybrid configuration via the introduction of N,S‐doped carbon substrate. The design leads to an enriched electron density around Fe active sites and significant reduction of energy barrier for OH* formation, which are favorable for the improvement of electrocatalytic ORR performance. This work provides a chance to expand the application of metallic macrocyclic compound electrocatalysts in various energy technologies.

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A Cu and Fe dual-atom nanozyme mimicking cytochrome c oxidase to boost the oxygen reduction reaction

Abstract: The intrinsically sluggish kinetics of oxygen reduction reaction (ORR) and overuse of expensive and unstable Pt-based catalysts have severely hampered the development of clean energy technologies. Herein, a type of...

Cited by 142 publications

References 48 publications

Atomically Dispersed Cu Nanozyme with Intensive Ascorbate Peroxidase Mimic Activity Capable of Alleviating ROS‐Mediated Oxidation Damage

Atomically Dispersed Cu Nanozyme with Intensive Ascorbate Peroxidase Mimic Activity Capable of Alleviating ROS‐Mediated Oxidation Damage

Fe‐ZIF8 Coating Cu Foil Derived Carbon as A pH‐Universal Electrocatalyst for Efficient Oxygen Reduction Reaction

Electronic Structure Regulation of Iron Phthalocyanine Induced by Anchoring on Heteroatom‐Doping Carbon Sphere for Efficient Oxygen Reduction Reaction and Al–Air Battery

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