The function-led design of porous hydrochar from mineral-rich biowaste for environmental applications inevitably suffers from carbon–ash recalcitrance. However, a method to alter the original carbon skeleton with ash remains elusive and hinders the availability of hydrochar. Herein, we propose a facile strategy for breaking the rigid structure of carbon–ash coupled hydrochar using phase-tunable molten carbonates. A case system was designed in which livestock manure and NaHCO were used to prepare the activated hydrochar, and NH served as the target contaminant. Due to the redox effect, we found that organic fractions significantly advanced the melting temperature of NaCO below 800 °C. The Na species steadily broke the carbon–ash interaction as the thermal intensity increased and transformed inorganic constituents to facilitate ash dissolution, rebuilding the hydrochar skeleton with abundant hierarchical channels and active defect edges. The surface polarity and mesopore distribution collectively governed the five cycles NH adsorption attenuation process. Manure hydrochar delivered favorable potential for application with a maximum overall adsorption capacity of 100.49 mg·g. Integrated spectroscopic characterization and theoretical computations revealed that incorporating NH on the carbon surface could transfer electrons to chemisorbed oxygen, which promoted the oxidation of pyridine-N during adsorption. This work offers deep insight into the structure-function correlation of hydrochar and inspires a more rational design of engineered hydrochar from high-ash biowaste.

中文翻译：

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通过熔融碳酸盐突破水热炭中的碳灰顽抗性：将富含矿物质的生物废物转化为可持续平台碳材料


以功能为主导的多孔水炭设计，以富含矿物质的生物废物为环境应用，不可避免地会受到碳灰顽抗的影响。然而，用灰分改变原始碳骨架的方法仍然难以捉摸，并阻碍了氢炭的可用性。在此，我们提出了一种使用相可调熔融碳酸盐打破碳灰耦合水热炭刚性结构的简单策略。设计了一个案例系统，其中牲畜粪便和 ​​NaHCO3 用于制备活性水炭，NH3 作为目标污染物。由于氧化还原效应，我们发现有机部分显着将 NaCO 的熔化温度提高到 800 °C 以下。随着热强度的增加，Na物种稳步打破碳-灰相互作用，并转化无机成分以促进灰溶解，重建具有丰富的分级通道和活性缺陷边缘的水炭骨架。表面极性和介孔分布共同控制了五个循环的NH吸附衰减过程。粪便水炭具有良好的应用潜力，最大总吸附容量为 100.49 mg·g。综合光谱表征和理论计算表明，在碳表面掺入NH可以将电子转移到化学吸附的氧上，从而促进吸附过程中吡啶-N的氧化。这项工作提供了对水炭结构与功能相关性的深入见解，并激发了对高灰分生物废物工程水炭进行更合理的设计。