Research Article Just Accepted
Synergy enhancement of Co single atoms and asymmetric sub-nanoclusters for Fenton-like activation
Nano Research
Available online: 29 May 2024
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As a new water treatment technology, Fenton-like reaction has great potential. In this study, we successfully prepared an excellent Fenton-like catalyst, which is composed of cobalt monoatoms and asymmetric subnanoclusters (labeled CoSA/Clu-C2N), and exhibits excellent peroxymonosulfate (PMS) activation reactivity. By directly comparing the catalytic properties of CoSA-C2N and CoSA/Clu-C2N, the synergistic effects of coasymmetric Co subclusters and Co atoms on the activation of PMS and degradation of organic micropollutants were investigated. The results showed that CoSA/Clu-C2N had higher degradation rates of CBZ, AT and CA when combined with active oxidant PMS. The cyclic frequency of Carbamazepine (CBZ) was 5.4 min-1, which was twice as high as the catalytic constant of CoSA-C2N (2.4 min-1). The results show that CoSA/Cul-C2N cobalt subnanoclusters and cobalt single atom can synergistically improve the catalytic performance of activated PMS oxidation of micropollutants in water. In addition, electron paramagnetic resonance (EPR) technology has proved that the introduction of Co subnano clusters in CoSA/Cu-C2N is conducive to the production of 1O2, thereby improving the efficiency of pollutant oxidation. This work lays a solid foundation for the future design of advanced multifunctional catalysts by carefully regulating and combining monmetallic atoms and metal subnanoclusters.

Research Article Issue
In situ reconstruction induced oxygen-deficient multiphase Cu based species hybridized with Ni single atoms as tandem platform for CO2 electroreduction
Nano Research 2024, 17 (5): 3888-3894
Published: 29 December 2023
Abstract PDF (15.2 MB) Collect

Tandem catalysis, capable of decoupling individual steps, provides a feasible way to build a high-efficiency CO2 electro-conversion system for multicarbons (C2+). The construction of electrocatalytic materials is one of focusing issues. Herein, we fabricated a single atom involved multivalent oxide-derived Cu composite material and found it inclined to reconstruct into oxygen-deficient multiphase Cu based species hybridized with monatomic Ni on N doped C matrix. In this prototype, rapid CO generation and C−C coupling are successively achieved on NiN4 sites and surface amorphized Cu species with defects, resembling a micro-production line. In this way, the in situ formed tandem catalyst exhibited a high Faradaic efficiency (FE) of ~ 78% for C2+ products along with satisfactory durability over 50 h. Particularly, the reconstruction-induced amorphous layer with abundant asymmetric sites should be favorable to improve the ethanol selectivity (FE: 63%), which is about 10 times higher than that of the non-tandem Cu-based contrast material. This work offers a new approach for manipulating tandem catalyst systems towards enhancing C2+ products.

Review Article Issue
Atomic interface regulation of rare-marth metal single atom catalysts for energy conversion
Nano Research 2024, 17 (5): 3493-3515
Published: 02 December 2023
Abstract PDF (18.2 MB) Collect

Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues. In recent years, with the rapid development of emerging catalysts, significant progress has been made in photocatalysis for converting solar energy into chemical energy and electrocatalysis for converting electrical energy into chemical energy. However, their selectivity and efficiency of the products are poor. Rare earth (RE) can achieve atomic level fine regulation of catalysts and play an crucial role in optimizing catalyst performance by their unique electronic and orbital structures. However, there is a lack of systematic review on the atomic interface regulation mechanism of RE and their role in energy conversion processes. Single atom catalysts (SACs) provide clear active sites and 100% atomic utilization, which is conducive to exploring the regulatory mechanisms of RE. Therefore, this review mainly takes atomic level doped RE as an example to review and discuss the atomic interface regulation role of RE elements in energy conversion. Firstly, a brief introduction was given to the synthesis strategies that can effectively exert the atomic interface regulation effect of RE, with a focus on the atomic interface regulation mechanism of RE. Meanwhile, the regulatory mechanisms of RE atoms have been systematically summarized in various energy conversion applications. Finally, the challenges faced by RE in energy conversion, as well as future research directions and prospects, were pointed out.

Research Article Issue
Interface electronic engineering of molybdenum sulfide/MXene hybrids for highly efficient biomimetic sensors
Nano Research 2023, 16 (1): 1158-1164
Published: 24 October 2022
Abstract PDF (18.8 MB) Collect

Interface regulation plays a key role in the electrochemical performance for biosensors. By controlling the interfacial interaction, the electronic structure of active species can be adjusted effectively at micro and nano-level, which results in the optimal reaction energy barrier. Herein, we propose an interface electronic engineering scheme to design a strongly coupled 1T phase molybdenum sulfide (1T-MoS2)/MXene hybrids for constructing an efficient electrocatalytic biomimetic sensor. The local electronic and atomic structures of the 1T-MoS2/Ti3C2TX are comprehensively studied by synchrotron radiation-based X-ray photoelectron spectroscopy (XPS), as well as X-ray absorption spectroscopy (XAS) at atomic level. Experiments and theoretical calculations show that there are interfacial stresses, atomic defects and adjustable bond-length between MoS2/MXene nanosheets, which can significantly promote biomolecular adsorption and rapid electron transfer to achieve excellent electrochemical activity and reaction kinetics. The 1T-MoS2/Ti3C2TX modified electrode shows ultra high sensitivity of 1.198 μA/μM for dopamine detection with low limit of 0.05 μM. We anticipate that the interface electronic engineering investigation could provide a basic idea for guiding the exploration of advanced biosensors with high sensitivity and low detection limit.

Research Article Issue
Dual single-atom Ce-Ti/MnO2 catalyst enhances low-temperature NH3-SCR performance with high H2O and SO2 resistance
Nano Research 2023, 16 (1): 299-308
Published: 11 August 2022
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Mn-based catalysts have exhibited promising performance in low-temperature selective catalytic reduction of NOx with NH3 (NH3-SCR). However, challenges such as H2O- or SO2-induced poisoning to these catalysts still remain. Herein, we report an efficient strategy to prepare the dual single-atom Ce-Ti/MnO2 catalyst via ball-milling and calcination processes to address these issues. Ce-Ti/MnO2 showed better catalytic performance with a higher NO conversion and enhanced H2O- and SO2-resistance at a low-temperature window (100−150 °C) than the MnO2, single-atom Ce/MnO2, and Ti/MnO2 catalysts. The in situ infrared Fourier transform spectroscopy analysis confirmed there is no competitive adsorption between NOx and H2O over the Ce-Ti/MnO2 catalyst. The calculation results showed that the synergistic interaction of the neighboring Ce-Ti dual atoms as sacrificial sites weakens the ability of the active Mn sites for binding SO2 and H2O but enhances their binding to NH3. The insight obtained in this work deepens the understanding of catalysis for NH3-SCR. The synthesis strategy developed in this work is easily scaled up to commercialization and applicable to preparing other MnO2-based single-atom catalysts.

Research Article Issue
Superoxide-like Cu/GO single-atom catalysts nanozyme with high specificity and activity for removing superoxide free radicals
Nano Research 2022, 15 (10): 8804-8809
Published: 26 July 2022
Abstract PDF (6.4 MB) Collect

Although nanozyme has become an emerging area of research attracting extensive attention recently, the activity and specificity of currently reported nanozymes are generally lower than those of natural enzymes. Developing highly active and specific nanozymes is therefore extremely necessary and also remains a great challenge. Superoxide dismutase (SOD) catalyzes the disproportionation of cytotoxic O2·− into hydrogen peroxide and oxygen, and plays an important role in reducing human oxidative stress. In this work, we prepare Cu single-atom catalysts (Cu/GO SACs, GO = graphene oxide) through a simple and low-cost strategy at room temperature using Cu foam and graphene oxide. Cu/GO SACs can maintain excellent catalytic activity under harsh environment. Compared with the natural enzyme, SOD-like Cu/GO SAC nanozyme has higher catalytic activity and meanwhile, it does not possess the common properties of other mimic enzymes often existing in nanomaterials. Based on the excellent SOD-like enzyme activity of Cu/GO SACs, it successfully eliminates the active oxygen in cigarette smoke. This work not only provides a new idea for the design and synthesis of nanozymes with excellent SOD mimetic properties, but also is promising in the treatment of lung injury and inflammatory diseases related to free radical production.

Research Article Issue
In situ decorating the surface and interlayer of montmorillonite with Co0.5Ni0.5Fe2O4 nanoparticles: A sustainable, biocompatible colorimetric platform for H2O2 and acetylcholine
Nano Research 2022, 15 (10): 9319-9326
Published: 24 June 2022
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Originated from nature and used for nature is a way of sustainable development. In this work, montmorillonite (MMT), a natural two-dimensional (2D) layered mineral, the surface and interlayer of which were nano-decorated by chemical synthesis technique was applied in biological detection field. Magnetic ferrite (Co0.5Ni0.5Fe2O4) was anchored on the surface and intercalated in the interlayer of montmorillonite, which served as a competitive candidate of enzyme mimics. Cytotoxicity test toward HUVEC and Hela cells verified the good biocompatibility of Co0.5Ni0.5Fe2O4-MMT, guaranteeing its safety in biological applications. Based on the peroxidase-like activity of Co0.5Ni0.5Fe2O4-MMT, a colorimetric sensing platform for H2O2 was established by a facile mix-and-detect approach with the detection limit of 0.565 μM (3σ/slope). It was implied that the peroxidase-like activity of Co0.5Ni0.5Fe2O4-MMT was originated from generation of ·OH and ·O2 produced from catalytic decomposition process of H2O2. Coupled with cascaded catalytic reactions of ACh, a facile and efficient sensing platform for ACh with satisfactory anti-interference ability was established. Thus, all these remarkable features highlighted the superiority of Co0.5Ni0.5Fe2O4-MMT, and endowed it with a powerful competitiveness in the fields of environmental assessing, biosensing, and disease monitoring.

Research Article Issue
Interfacial engineering of 3D hollow CoSe2@ultrathin MoSe2 core@shell heterostructure for efficient pH-universal hydrogen evolution reaction
Nano Research 2022, 15 (4): 2895-2904
Published: 06 November 2021
Abstract PDF (9.6 MB) Collect

Rational design and construction of low-cost and highly efficient electrocatalysts for hydrogen evolution reaction (HER) is meaningful but challenging. Herein, a robust three dimensional (3D) hollow CoSe2@ultrathin MoSe2 core@shell heterostructure (CoSe2@MoSe2) is proposed as an efficient HER electrocatalyst through interfacial engineering. Benefitting from the abundant heterogeneous interfaces on CoSe2@MoSe2, the exposed edge active sites are maximized and the charge transfer at the hetero-interfaces is accelerated, thus facilitating the HER kinetics. It exhibits remarkable performance in pH-universal conditions. Notably, it only needs an overpotential (η10) of 108 mV to reach a current density of 10 mA·cm−2 in 1.0 M KOH, outperforming most of the reported transition metal selenides electrocatalysts. Density functional theory (DFT) calculations unveil that the heterointerfaces synergistically optimize the Gibbs free energies of H2O and H* during alkaline HER, accelerating the reaction kinetics. The present work may provide new construction guidance for rational design of high-efficient electrocatalysts.

Review Article Issue
Rational design of Fe-N-C electrocatalysts for oxygen reduction reaction: From nanoparticles to single atoms
Nano Research 2022, 15 (3): 1753-1778
Published: 18 September 2021
Abstract PDF (24.6 MB) Collect

As an alternative energy, hydrogen can be converted into electrical energy via direct electrochemical conversion in fuel cells. One important drawback of full cells is the sluggish oxygen reduction reaction (ORR) promoted by the high-loading of platinum-group-metal (PGM) electrocatalysts. Fe-N-C family has been received extensive attention because of its low cost, long service life and high oxygen reduction reaction activity in recent years. In order to further enhance the ORR activity, the synthesis method, morphology regulation and catalytic mechanism of the active sites in Fe-N-C catalysts are investigated. This paper reviews the research progress of Fe-N-C from nanoparticles to single atoms. The structure-activity relationship and catalytic mechanism of the catalyst are studied and discussed, which provide a guidance for rational design of the catalyst, so as to promote the more reasonable design of Fe-N-C materials.

Review Article Issue
Single atom catalysts by atomic diffusion strategy
Nano Research 2021, 14 (12): 4398-4416
Published: 07 April 2021
Abstract PDF (70.5 MB) Collect

The depletion of energy and increasing environmental pressure have become one of the main challenges in the world today. Synthetic high-efficiency catalysts bring hope for efficient conversion of energy and effective treatment of pollutants, especially, single-atom catalysts (SACs) are promising candidates. Herein, we comprehensively summarizes the atomic diffusion strategy, which is considered as an effective method to prepare a series of SACs. According to the different diffusion forms of the precursors, we review the synthesis pathways of SACs from three aspects: gas diffusion, solid diffusion and liquid diffusion. The gaseous diffusion method mainly discusses atomic layer deposition (ALD) and chemical vapor deposition (CVD), both of which carry out gas phase mass transfer at high temperatures. The solid-state diffusion method can be divided into nanoparticle transformation into single atoms and solid atom migration. Liquid diffusion mainly describes the electrochemical method and the molten salt method. We hope this review can trigger the rational design of SACs.

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