The solar‐driven photocatalytic reduction of CO2 (CO2RR) into chemical fuels is a promising route to enrich energy supplies and mitigate CO2 emissions. However, low catalytic efficiency and poor selectivity, especially in a pure‐water system, hinder the development of photocatalytic CO2RR owing to the lack of effective catalysts. Herein, we report a novel atom‐confinement and coordination (ACC) strategy to achieve the synthesis of rare‐earth single erbium (Er) atoms supported on carbon nitride nanotubes (Er1/CN‐NT) with a tunable dispersion density of single atoms. Er1/CN‐NT is a highly efficient and robust photocatalyst that exhibits outstanding CO2RR performance in a pure‐water system. Experimental results and density functional theory calculations reveal the crucial role of single Er atoms in promoting photocatalytic CO2RR.
Ionic-liquid gating on a functional thin film with a low voltage has drawn a lot of attention due to rich chemical, electronic, and magnetic phenomena at the interface. Here, a key challenge in quantitative determination of voltage-controlled magnetic anisotropy (VCMA) in Au/[DEME] [TFSI] /Co field-effect transistor heterostructures is addressed. The magnetic anisotropy change as response to the gating voltage is precisely detected by in situ electron spin resonance measurements. A reversible change of magnetic anisotropy up to 219 Oe is achieved with a low gating voltage of 1.5 V at room temperature, corresponding to a record high VCMA coefficient of ≈146 Oe V . Two gating effects, the electrostatic doping and electrochemical reaction, are distinguished at various gating voltage regions, as confirmed by X-ray photoelectron spectroscopy and atomic force microscopy experiments. This work shows a unique ionic-liquid-gating system for strong interfacial magnetoelectric coupling with many practical advantages, paving the way toward ion-liquid-gating spintronic/electronic devices.
One of the central challenges in realizing multiferroics-based magnetoelectric memories is to switch perpendicular magnetic anisotropy (PMA) with a control voltage. In this study, we demonstrate electrical flipping of magnetization between the out-of-plane and the in-plane directions in (Co/Pt)/(011) Pb(MgNb)O-PbTiO multiferroic heterostructures through a voltage-controllable spin reorientation transition (SRT). The SRT onset temperature can be dramatically suppressed at least 200 K by applying an electric field, accompanied by a giant electric-field-induced effective magnetic anisotropy field (ΔH) up to 1100 Oe at 100 K. In comparison with conventional strain-mediated magnetoelastic coupling that provides a ΔH of only 110 Oe, that enormous effective field is mainly related to the interface effect of electric field modification of spin-orbit coupling from Co/Pt interfacial hybridization via strain. Moreover, electric field control of SRT is also achieved at room temperature, resulting in a ΔH of nearly 550 Oe. In addition, ferroelastically nonvolatile switching of PMA has been demonstrated in this system. E-field control of PMA and SRT in multiferroic heterostructures not only provides a platform to study strain effect and interfacial effect on magnetic anisotropy of the ultrathin ferromagnetic films but also enables the realization of power efficient PMA magnetoelectric and spintronic devices.
The configuration regulation of single‐atom photocatalysts (SAPCs) can significantly influence the interfacial charge transfer and subsequent catalytic process. The construction of conventional SAPCs for aqueous CO2 reduction is mainly devoted toward favorable activation and photoreduction of CO2, however, the role of water is frequently neglected. In this work, single Ni atoms are successfully anchored by boron‐oxo species on g‐C3N4 nanosheets through a facile ion‐exchange method. The dative interaction between the B atom and the sp2 N atom of g‐C3N4 guarantees the high dispersion of boron‐oxo species, where O atoms coordinate with single Ni (II) sites to obtain a unique six‐oxygen‐coordinated configuration. The optimized single‐atom Ni photocatalyst, rivaling Pt‐modified g‐C3N4 nanosheets, provides excellent CO2 reduction rate with CO and CH4 as products. Quasi‐in‐situ X‐ray photoelectron spectra, transient absorption spectra, isotopic labeling, and in situ Fourier transform infrared spectra reveal that as‐fabricated six‐oxygen‐coordinated single Ni (II) sites can effectively capture the photoelectrons of CN along the BO bridges and preferentially activate adsorbed water to produce H atoms to eventually induce a hydrogen‐assisted CO2 reduction. This work diversifies the synthetic strategies for single‐atom catalysts and provides insight on correlation between the single‐atom configuration and reaction pathway.
A universal strategy is developed to construct a cascade Z‐Scheme system, in which an effective energy platform is the core to direct charge transfer and separation, blocking the unexpected type‐II charge transfer pathway. The dimension‐matched (001)TiO2‐g‐C3N4/BiVO4 nanosheet heterojunction (T‐CN/BVNS) is the first such model. The optimized cascade Z‐Scheme exhibits ≈19‐fold photoactivity improvement for CO2 reduction to CO in the absence of cocatalysts and costly sacrificial agents under visible‐light irradiation, compared with BVNS, which is also superior to other reported Z‐Scheme systems even with noble metals as mediators. The experimental results and DFT calculations based on van der Waals structural models on the ultrafast timescale reveal that the introduced T as the platform prolongs the lifetimes of spatially separated electrons and holes and does not compromise their reduction and oxidation potentials.
We report electric-field control of magnetism of (Co/Pt) multilayers involving perpendicular magnetic anisotropy with different Co-layer thicknesses grown on Pb(Mg,Nb)O-PbTiO (PMN-PT) FE substrates. For the first time, electric-field control of the interface magnetic anisotropy, which results in the spin reorientation transition, was demonstrated. The electric-field-induced changes of the bulk and interface magnetic anisotropies can be understood by considering the strain-induced change of magnetoelastic energy and weakening of Pt 5d-Co 3d hybridization, respectively. We also demonstrate the role of competition between the applied magnetic field and the electric field in determining the magnetization of the sample with the coexistence phase. Our results demonstrate electric-field control of magnetism by harnessing the strain-mediated coupling in multiferroic heterostructures with perpendicular magnetic anisotropy and are helpful for electric-field modulations of Dzyaloshinskii-Moriya interaction and Rashba effect at interfaces to engineer new functionalities.
Die rationale Entwicklung effizienter Photokatalysatoren mit günstiger Ladungstrennung und breiter spektraler Absorption ist entscheidend für eine ökonomische Umwandlung von Solarenergie in chemische Energie. F. Q. Bai, J. Tang, L. Q. Jing et al. zeigen in ihrer Zuschrift auf S. 10989 H‐verbrückte ZnPc/BiVO4‐Nanokomposite als ultradünnen, räumlich angepassten 2D/2D‐Heteroübergang zur effizienten photokatalytischen CO2‐Reduktion über eine breite Region des sichtbaren Lichts.
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