Synergistically coupled 1D/2D materials have great potential for energy conversion application due to its high catalytic activity. Herein, an in situ assembly strategy is developed for preparing the P, N co‐doped carbon nanotubes and Mo/MoS_2(1−x−y)P_x nanosheets composites (Mo/MoS_2(1−x−y)P_x@PNC) for hydrogen evolution reactions (HER). The PNC guarantees structural stability and fast charge transfer in a long‐range, while Mo/MoS_2(1−x−y)P_x nanosheets offer a large electrochemically active surface area with embedded metallic Mo in improving its internal conductivity and rich surface/interface properties. Thus, the optimized catalyst (Mo/MoS_1.15P_0.30@PNC) possesses more surface active sites and exhibits extraordinary HER activities, with a small overpotential of −79 and −131 mV at 10 mA cm⁻¹, and low Tafel slope of 49 and 82 mV dec⁻¹ in 0.5 m H₂SO₄ and 1.0 m KOH, respectively. Density functional theory calculations confirm that the higher substitution of S atoms by P in MoS₂ can form strong Mo 3d‐S 2p‐P 2p hybridizations at Fermi level, resulting in the narrower bandgap and smaller ∆G_H* of hydrogen (H*) adsorption, thereby leading to the promoted HER activity.

中文翻译：

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P，N共掺杂碳纳米管上组装的分层超薄Mo / MoS2（1-x-y）Px纳米片用于在酸性和碱性电解质中析氢

协同耦合的1D / 2D材料由于其高催化活性而具有巨大的能量转化应用潜力。本文提出了一种原位组装策略，用于制备P，N共掺杂的碳纳米管和Mo / MoS _{2（1- x - y）} P _x纳米片复合材料（Mo / MoS _{2（1- x - y）} P _x @PNC）用于析氢反应（HER）。PNC保证了结构稳定性和长距离的快速电荷转移，而Mo / MoS _{2（1- x - y）} P _x纳米片具有较大的电化学活性表面积，其中嵌入了金属Mo，可改善其内部电导率和丰富的表面/界面特性。因此，优化的催化剂（Mo / MoS _1.15 P _0.30 @PNC）具有更多的表面活性位点，并展现出非凡的HER活性，在10 mA cm ^-1时具有-79和-131 mV的小超电势，且Tafel斜率低至49分别在0.5 m H ₂ SO ₄和1.0 m KOH中为82 mV dec ^-1。密度泛函理论计算证实了MoS _2中P取代S原子的程度更高可以在费米能级上形成强烈的Mo 3d-S 2p-P 2p杂化，导致带隙更窄，氢（H *）吸附的ΔG _{H *}较小，从而导致HER活性增强。