Constrain nickel bicarbonate within Ni-modified graphitized carbonized wood for efficient urea electro-oxidation

IF 5.4 2区化学 Q2 CHEMISTRY, PHYSICAL

Colloids and Surfaces A: Physicochemical and Engineering Aspects Pub Date : 2026-05-20 Epub Date: 2026-02-08 DOI:10.1016/j.colsurfa.2026.139889

Jixin Peng , Can Sheng , Xinya Ye , Han Xu , Duping Wang , Kang Xu , Yuanyuan Liao , Yan Qing , Yiqiang Wu

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Abstract

The practical implementation of urea oxidation reaction (UOR) for energy-saving hydrogen generation is hindered by the lack of efficient and robust non-precious electrocatalysts. Herein, we design a novel hybrid catalyst comprising nickel bicarbonate anchored on a Ni-modified graphitized carbonized wood substrate (Ni(HCO₃)₂-Ni/GCW). This architecture effectively overcomes the inherent kinetic limitations and stability challenges of UOR. The hierarchical porous network of the wood-derived carbon facilitates superior mass transport and exposes numerous sites for catalyst loading. Advanced characterization and density functional theory computations uncover the pivotal role of carbonate groups in Ni(HCO₃)₂, which function as non-innocent ligands to strengthen urea adsorption and ease CO₂ product release, thereby significantly elevating UOR activity. Ni(HCO₃)₂-Ni/GCW combines a low UOR potential of 1.34 V (vs. RHE at 50 mA·cm⁻²) with outstanding operational stability. When assembled for overall urea splitting, the Pt/C||Ni(HCO₃)₂-Ni/GCW electrolyzer operates at 1.59 V to deliver 50 mA·cm⁻², achieving a notable 230 mV reduction in the cell voltage relative to conventional water splitting (1.82 V). This research establishes a new paradigm for engineering stable and highly active UOR catalysts through the strategic integration of functional materials with renewable biomass-derived scaffolds.

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在镍改性石墨化碳化木材中约束碳酸氢镍，以实现高效的尿素电氧化

由于缺乏高效、稳定的非贵重电催化剂，阻碍了尿素氧化反应节能制氢的实际实施。在此，我们设计了一种新型的混合催化剂，该催化剂由碳酸氢镍锚定在镍改性的石墨化碳化木材基体（Ni(HCO3)2-Ni/GCW）上。这种结构有效地克服了UOR固有的动力学限制和稳定性挑战。木材衍生碳的分层多孔网络促进了优越的质量运输，并暴露了许多催化剂负载的场所。先进的表征和密度功能理论计算揭示了碳酸盐基团在Ni(HCO3)2中的关键作用，它们作为非无害配体加强尿素吸附和减缓CO2产物释放，从而显著提高UOR活性。Ni(HCO3)2-Ni/GCW结合了1.34 V的低UOR电位（相对于50 mA·cm−2的RHE）和出色的操作稳定性。当组装用于整体尿素分解时，Pt/C||Ni(HCO3)2-Ni/GCW电解槽在1.59 V下工作，输出50 mA·cm - 2，相对于传统的水分解（1.82 V），电池电压显著降低230 mV。本研究通过功能材料与可再生生物质衍生支架的战略性整合，为工程稳定和高活性的UOR催化剂建立了新的范例。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Colloids and Surfaces A: Physicochemical and Engineering Aspects 化学-物理化学

CiteScore

8.70

自引率

9.60%

发文量

2421

审稿时长

56 days

期刊介绍： Colloids and Surfaces A: Physicochemical and Engineering Aspects is an international journal devoted to the science underlying applications of colloids and interfacial phenomena. The journal aims at publishing high quality research papers featuring new materials or new insights into the role of colloid and interface science in (for example) food, energy, minerals processing, pharmaceuticals or the environment.