The origin of selective adsorption desulfurization by Fe single atom adsorbents on hexagonal boron nitride surface

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-11-21 DOI:10.1016/j.seppur.2024.130641

Naixia Lv, Tianxiao Zhu, Dongmei Luo, Wei Yi, Chunyan Dai, Hongping Li, Wenshuai Zhu, Huaming Li

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Abstract

Hexagonal boron nitride (h-BN) has widespread application in the field of adsorption desulfurization due to their excellent performance. However, the selective adsorption of h-BN is still a challenge. Here, to further enhance the adsorption capacity and selectivity of BN-based adsorbents, the stability of Fe single-atom adsorbents (SAAs, Fe-BN), and their adsorption performance and mechanism towards the representative sulfide, dibenzothiophene (DBT) were investigated by density functional theory calculations. Specifically, four Fe doping types are considered: Fe_cen_B and Fe_edg_B (both at B sites), Fe_cen_N (at the N site), and Fe_four_cen (at the B − N site). All types of Fe-BN SAAs exhibit outstanding adsorption capacity for thiophenic sulfides. Especially for Fe_edg_B1, which shows 62.6 % improvement in adsorption performance compared to h-BN for DBT. Quantum chemical analysis reveals that S-Fe coordination bonds formed between S atom in DBT and Fe atoms via coordination interaction, significantly improving the adsorption selectivity and capacity. This study may provide a useful reference for designing the highly selective SAAs.

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六方氮化硼表面铁单原子吸附剂选择性吸附脱硫的起源

六方氮化硼（h-BN）因其优异的性能在吸附脱硫领域得到了广泛应用。然而，h-BN 的选择性吸附仍然是一个难题。为了进一步提高 BN 基吸附剂的吸附能力和选择性，本文通过密度泛函理论计算研究了铁单原子吸附剂（SAAs，Fe-BN）的稳定性及其对代表性硫化物二苯并噻吩（DBT）的吸附性能和机理。具体来说，我们考虑了四种铁掺杂类型：Fe_cen_B和Fe_edg_B（均位于B位）、Fe_cen_N（位于N位）和Fe_four_cen（位于B - N位）。所有类型的 Fe-BN SAA 对噻吩硫化物都有出色的吸附能力。特别是 Fe_edg_B1，与 h-BN 相比，它对 DBT 的吸附性能提高了 62.6%。量子化学分析表明，DBT 中的 S 原子与 Fe 原子通过配位相互作用形成了 S-Fe 配位键，从而显著提高了吸附选择性和吸附容量。这项研究可为设计高选择性的 SAAs 提供有益的参考。

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

Separation and Purification Technology 工程技术-工程：化工

CiteScore

14.00

自引率

12.80%

发文量

2347

审稿时长

43 days

期刊介绍： Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.