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Hydrogen evolution reaction (HER) catalysts based on noble metals traditionally suffered from high cost, low activity, and poor stability. Metal-free catalysts originating from heteroatom-doped carbon materials have been proposed to address these problems, in which the doping configurations and electronic structures are critical for modulating the electrocatalytic activity. Herein, we reported a sequential approach for the co-doping of B and N atoms into graphdiyne (GDY). We noticed that the configurations of heteroatoms are strongly related to the doping process, and the subsequent HER test shows that a certain sp-N can decrease the overpotential, and further introduction of B atoms can continuously enhance the current density owing to the synergistic effect of chemical and electronic couplings on proton adsorption/reduction kinetics. This work provides a deeper understanding of developing dual heteroatom doped non-metallic catalysts. [ABSTRACT FROM AUTHOR]

In the study of structure–property relationships for rational materials design, hollow multishell structures (HoMSs) have attracted tremendous attention owing to the optimal balance between mass transfer and surface exposure. Considering the shell structure can significantly affect the properties of HoMSs, in this paper, we provide a novel one‐step strategy to continually regulate the shell structures of HoMSs. Through a simple phosphorization process, we can effectively modify the shell from solid to bubble‐like and even duplicate the shells with a narrow spacing. Benefitting from the structure merits, the fabricated CoP HoMSs with close duplicated shells can promote gas release owing to the unbalanced Laplace pressure, while accelerating liquid transfer for enhanced capillary force. It can provide effective channels for water and gas and thus exhibits a superior electrocatalytic performance in the hydrogen and oxygen evolution reaction. [ABSTRACT FROM AUTHOR]

To boost the performance for various applications, a rational bottom‐up design on materials is necessary. The defect engineering on nanoparticle at the atomic level can efficiently tune the electronic behavior, which offers great opportunities in enhancing the catalytic performance. In this paper, we optimized the surface oxygen vacancy concentration and created the lattice distortion in rare‐earth‐based perovskite oxide through gradient replacement of the B site with valence alternated element. The dual defects make the electron spin state transit from low spin state to high spin state, thus decreasing the charge transport resistance. Furthermore, assembly the modified nanoparticle subunits into the micro‐sized hollow multishelled structures can provide porous shells, abundant interior space and effective contact, which enables an enhanced mass transfer and a shorter charge transport path. As a result, the systemic design in the electronic and nano‐micro structures for catalyst has brought an excellent oxygen evolution performance. [ABSTRACT FROM AUTHOR]

The crystal phase plays an important role in controlling the properties of a nanomaterial; however, it is a great challenge to obtain a nanomaterial with high purity of the metastable phase. For instance, the large‐scale synthesis of the metallic phase MoS2 (1T‐MoS2) is important for enhancing electrocatalytic reaction, but it can only be obtained under harsh conditions. Herein, a spatially confined template method is proposed to synthesize high phase‐purity MoS2 with a 1T content of 83 %. Moreover, both the confined space and the structure of template will affect the purity of 1T‐MoS2; in this case, this approach was extended to other similar spatially confined templates to obtain the high‐purity material. The obtained ultrathin nanosheets exhibit good electrocatalytic activity and excellent stability in the hydrogen evolution reaction. [ABSTRACT FROM AUTHOR]