过渡金属修饰的氮改性碳纳米带储氢性能
Hydrogen Storage on Transition-Metal-Decorated Nitrogen-Modified Carbon Nanoribbons
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中文总结 AI 辅助
该研究通过第一性原理计算，用Mn和Y掺杂氮改性碳纳米带，使储氢性能达到美国能源部要求，其中Mn掺杂体系在近环境工况下仍保持7.48 wt%的储氢容量。
中文摘要 AI 辅助
采用第一性原理密度泛函理论计算，对近期合成的碳纳米带（CNRs）的储氢性能展开研究。本征CNRs对H₂的吸附作用较弱，因此通过在C-H边缘用12个氮原子取代碳原子对主体结构进行改性，随后掺杂锰（Mn）和钇（Y）以增强H₂的结合作用；12N-CNRs上最多可容纳5个金属原子。电子结构分析显示金属原子与CNRs间存在强轨道杂化，结合能计算证实了掺杂体系的结构稳定性；Bader电荷分析进一步量化了金属原子与主体结构间的电荷转移。计算得出Mn掺杂体系的平均H₂吸附能为-0.40 eV/H₂，Y掺杂体系为-0.25 eV/H₂，二者均处于可逆储氢所需的理想范围内。在0 K条件下，Mn掺杂体系的最大理论重量储氢容量达7.48 wt%，Y掺杂体系为6.55 wt%；在30 atm、298.15 K的实际工况下，Y掺杂体系的储氢容量降至6.04 wt%，而Mn掺杂体系则保持7.48 wt%的全容量。热力学分析表明，低温高压有利于H₂吸附，高温低压则使脱附成为可能。上述结果表明，Mn和Y掺杂的CNRs满足美国能源部对可逆储氢的关键要求，有望成为近环境条件下的潜在储氢材料。
英文摘要
Recently synthesized carbon nanoribbons (CNRs) were investigated for hydrogen (H2) storage using first-principles density functional theory calculations. Pristine CNRs exhibited weak H2 adsorption; therefore, the host structure was modified by substituting carbon atoms at the C-H edges with 12 nitrogen atoms, followed by Mn and Y doping to enhance H2 binding. A maximum of five metal atoms could be accommodated on the 12N-CNRs. Electronic structure analysis revealed strong orbital hybridization between the metal atoms and the CNRs, while binding energy calculations confirmed the structural stability of the doped systems. Bader charge analysis further quantified the charge transfer between the metal atoms and the host structure. The average H2 adsorption energies were calculated to be -0.40 eV/H2 for the Mn-doped system and -0.25 eV/H2 for the Y-doped system, which are within the desirable range for reversible hydrogen storage. The maximum theoretical gravimetric storage capacities at 0 K reached 7.48 wt% for the Mn-doped system and 6.55 wt% for the Y-doped system. Under practical conditions of 30 atm and 298.15 K, the storage capacity of the Y-doped system decreased to 6.04 wt%, whereas the Mn-doped system maintained its full capacity of 7.48 wt%. Thermodynamic analysis indicated that H2 adsorption is favored at low temperatures and high pressures, while desorption becomes feasible at elevated temperatures and lower pressures. These results demonstrate that Mn- and Y-doped CNRs satisfy key U.S. Department of Energy requirements for reversible H2 storage and show promise as potential hydrogen storage materials under near-ambient conditions.
发表机构
- University of New England（新英格兰大学）
- Karpagam Academy of Higher Education（卡尔帕甘高等教育学院）
- Bhabha Atomic Research Centre（巴哈原子研究中心）
- Homi Bhabha National Institute（霍米·巴巴国立研究所）
- University of Canberra（堪培拉大学）
- The University of Queensland（昆士兰大学）
机构由 AI 辅助整理，请以论文原文为准。
