Modulating the electronic structure of ternary transition metal phosphide for enhanced hydrogen evolution activity,Dalton Transactions

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Modulating the electronic structure of ternary transition metal phosphide for enhanced hydrogen evolution activity
Dalton Transactions ( IF 3.5 ) Pub Date : 2022-11-16 , DOI: 10.1039/d2dt03083g
Sheying Dong ₁ , Huangcong Tang ₁ , Kangkang Wang ₁ , Qian Zheng ₁ , Tinglin Huang ₂

Affiliation

Rationally designing ternary transition-metal phosphides (TMPs) for the hydrogen evolution reaction (HER) is desirable but remains a significant challenge. Herein, ternary FeCoNiP encapsulated in a porous carbon shell, coupled with N-doped carbon nanotubes (FeCoNiP@NCNTs) are synthesized via a simple pyrolysis–phosphatization strategy derived from FeCoNi-MOF-100@dicyandiamide. Because Co/Ni enters the FeP lattice, FeCoNiP@NCNTs show a favorable catalytic performance towards the HER with low overpotential values of 86.7 and 233.5 mV at 10 mA cm⁻² in acidic and alkaline media, respectively, surpassing the HER performance of FeP@NCNTs, FeCoP@NCNTs, and FeNiP@NCNTs. Impressively, FeCoNiP@NCNTs display adequate acid-resistance capacity during the HER process, with nearly negligible decay due to the thin graphitized carbon shell structure with a thickness of 11.5–20.3 nm. The results of experiments, structural characterization, and density functional theory (DFT) calculations demonstrate that Co/Ni co-doping can modulate the adsorption and dissociation processes of H⁺ and downshift the d-band center of FeP. This work proposes a strategy for fabricating ternary TMP catalysts with heterogeneous structures for the HER.

中文翻译：

调节三元过渡金属磷化物的电子结构以增强析氢活性

合理设计用于析氢反应 (HER) 的三元过渡金属磷化物 (TMP) 是可取的，但仍然是一个重大挑战。在此，封装在多孔碳壳中的三元 FeCoNiP 与 N 掺杂碳纳米管 (FeCoNiP@NCNTs)通过源自 FeCoNi-MOF-100@双氰胺的简单热解-磷酸化策略合成。由于 Co/Ni 进入 FeP 晶格，FeCoNiP@NCNTs 对 HER 表现出良好的催化性能，在 10 mA cm ^{-2时具有 86.7 和 233.5 mV 的低过电位值}在酸性和碱性介质中，分别超过了 FeP@NCNTs、FeCoP@NCNTs 和 FeNiP@NCNTs 的 HER 性能。令人印象深刻的是，FeCoNiP@NCNTs 在 HER 过程中显示出足够的耐酸能力，由于厚度为 11.5-20.3 nm 的薄石墨化碳壳结构，衰减几乎可以忽略不计。实验、结构表征和密度泛函理论 (DFT) 计算的结果表明，Co/Ni 共掺杂可以调节 H ⁺的吸附和解离过程，并使 FeP 的 d 带中心下移。这项工作提出了一种为 HER 制造具有多相结构的三元 TMP 催化剂的策略。

更新日期：2022-11-16

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