Over the years, transition metal-based hybrids have been advocated as one of the most promising classes of non-noble catalysts and investigated exclusively for the electrocatalytic triiodide reduction reaction (IRR) or hydrogen evolution reaction (HER). However, there is lack of effective strategy to address their site accessibility, intrinsic activity and structural stability issues, and their successful utilization as bifunctional catalysts of IRR and HER is rarely explored. Herein, presented is a multimetal-based carbon nanotube hybrid (CoFeNiMo@NCNT), synthesized from a novel polyoxometalate (POM)-intercalated layered double hydroxide (LDH) pyrolysis strategy, as an efficient catalyst for IRR and HER. During both electrochemical IRR and HER, the regulated NCNT provides a highway for electron migration and acts as a network for I₃⁻/H⁺ adsorption. Benefitting from the features of porous structure, multimetal component and fast electron transfer, the CoFeNiMo@NCNT catalyst delivers a high power conversion efficiency of 6.46 % when assembled as counter electrode in dye-sensitized solar cell, superior to Pt benchmark. Furthermore, it mediates efficient HER with a relatively small overpotential of 209.9 mV at 10 mA cm^-2. The strategy to achieve tunable catalytic properties via in situ pyrolysis well-defined inorganic materials paves a new way to design cost-effective and efficient bifunctional catalysts.

多年来，基于过渡金属的杂化物已被提倡为最有前景的非贵金属催化剂之一，并专门针对电催化三碘化物还原反应（IRR）或析氢反应（HER）进行了研究。然而，缺乏有效的策略来解决它们的位点可及性，内在活性和结构稳定性问题，并且很少探索将其成功地用作IRR和HER的双功能催化剂。在这里，提出了一种基于多金属的碳纳米管杂化物（CoFeNiMo @ NCNT），它是由一种新型的多金属氧酸盐（POM）插入层状双氢氧化物（LDH）热解策略合成的，作为IRR和HER的有效催化剂。在电化学IRR和HER期间，受调节的NCNT为电子迁移提供了一条高速公路，并充当了I₃ ^- / H ⁺吸附。得益于多孔结构，多金属组分和快速电子转移的特点，CoFeNiMo @ NCNT催化剂作为染料敏化太阳能电池的对电极组装时，可实现6.46％的高功率转换效率，优于Pt基准。此外，它介导有效的HER，在10 mA cm ^-2时具有209.9 mV的相对较小的过电势。通过原位热解获得明确的无机材料实现可调节的催化性能的策略为设计经济高效的双功能催化剂开辟了一条新途径。