The pursuit of multifunctional electrocatalysts holds significant importance due to their comprehension of material chemistry. Amorphous materials are particularly appealing, yet they pose challenges in terms of rational design due to their structural disorder and thermal instability. Herein, we propose a strategy that entails the tandem (low-temperature/250–350 °C) pyrolysis of molecular clusters, enabling preservation of the local short-range structures of the precursor Schiff base nickel (Ni₃[2(C₂₁H₂₄N₃Ni_1.5O₆)]). The temperature-dependent residuals demonstrate exceptional activity and stability for at least three distinct electrocatalytic processes, including the oxygen evolution reaction (η₁₀ = 197 mV), urea oxidation reaction (η₁₀ = 1.339 V), and methanol oxidation reaction (1358 mA cm⁻² at 0.56 V). Three distinct nickel atom motifs are discovered for three efficient electrocatalytic reactions (Ni1 and Ni1′ are preferred for UOR/MOR, while Ni2 is preferred for OER). Our discoveries pave the way for the potential development of multifunctional electrocatalysts through disordered engineering in molecular clusters under tandem pyrolysis.

中文翻译：

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热解对称三核镍簇中的非晶转化触发三功能电催化剂

由于对材料化学的理解，对多功能电催化剂的追求具有重要意义。非晶材料特别有吸引力，但由于其结构无序和热不稳定，给合理设计带来了挑战。在此，我们提出了一种策略，该策略需要分子簇的串联（低温/250–350°C）热解，从而能够保留前体席夫碱镍（Ni ₃ [2(C ₂₁ H）₂₄ N ₃ Ni _1.5 O ₆ )])。与温度相关的残差在至少三种不同的电催化过程中表现出优异的活性和稳定性，包括析氧反应（η ₁₀ = 197 mV）、尿素氧化反应（η ₁₀ = 1.339 V）和甲醇氧化反应（1358 mA cm）⁻²（0.56V）。三个不同的镍原子基序被发现可用于三种有效的电催化反应（UOR/MOR 首选 Ni1 和 Ni1'，而 OER 首选 Ni2）。我们的发现为通过串联热解下分子簇的无序工程开发多功能电催化剂的潜力铺平了道路。