Highly Sensitive and Selective Zinc-Based Metal-Organic Framework Derivatives Gas Sensors for Trace H2S Detection.

IF 9.1 1区 化学 Q1 CHEMISTRY, ANALYTICAL
Wei Wang,Li Chen,Leif Riemenschneider,Chen-Chen Wang,Luis-Antonio Panes-Ruiz,Martin Hantusch,Yun-Xu Chen,Jian-Jun Zhang,Shivam Singh,Yana Vaynzof,Markus Löffler,Arezoo Dianat,Naisa Chandrasekhar,Shi-Rong Huang,Gianaurelio Cuniberti
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Abstract

High sensitivity and selectivity are never-ending points of interest in the gas sensing field. Herein, the novel functionalized N-doped graphitic carbon is derived from Zn-MOF by modulating the pyrolysis temperature toward H2S sensing application. The results demonstrate excellent sensing performance toward H2S gas with a limit of detection (LOD) of 56.9 ppb, faster response and recovery time (18 and 29 s), and high selectivity with a 20-fold response difference than other interfering gases. The expected stability with stable multiple consecutive responses and a strong response toward 1 ppm of H2S after 4 months were reached. Functionalized groups pyridinic nitrogen (PD-N) and pyrrolic nitrogen (PR-N) that make MOF-derived carbon stand out in H2S gas sensing are mainly attributed to dual active sites: (i) N-C bonds on graphitic carbon undergo surface redox reactions, forming oxidized carbon species (C═O or C═S), and (ii) PD/PR-N-Zn coordination centers facilitate the formation of SO42--based surface complexes through reaction with H2S and adsorbed oxygen. Notably, DFT calculation was employed to confirm both PR-N and PD-N bonding with zinc, yielding the largest charge transfer and binding energy among simulated factors, which attributes to the generation of significant sensing performance for H2S. Consequently, this work will provide a novel strategy for the advancement of gas sensing applications.
用于痕量H2S检测的高灵敏度和选择性锌基金属-有机框架衍生物气体传感器。
高灵敏度和高选择性是气体传感领域永无止境的研究热点。本文通过对Zn-MOF热解温度的调节,制备了新型功能化n掺杂石墨碳,并将其应用于H2S传感。结果表明,该传感器对H2S气体具有良好的传感性能,检出限为56.9 ppb,响应时间和恢复时间分别为18 s和29 s,选择性高,响应差为其他干扰气体的20倍。达到了预期的稳定性,稳定的多次连续响应和4个月后对1 ppm H2S的强烈响应。使mof衍生碳在H2S气敏中脱颖而出的功能化基团吡啶氮(PD- n)和吡啶氮(PR-N)主要归因于双活性位点:(i)石墨碳上的N-C键进行表面氧化还原反应,形成氧化碳种(C = O或C = S), (ii) PD/PR-N- zn配位中心通过与H2S和吸附氧的反应促进形成SO42-表面配合物。值得注意的是,DFT计算证实了PR-N和PD-N与锌的键合,在模拟因子中产生的电荷转移和结合能最大,这归因于对H2S产生了显著的传感性能。因此,这项工作将为气体传感应用的进步提供一种新的策略。
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
ACS Sensors
ACS Sensors Chemical Engineering-Bioengineering
CiteScore
14.50
自引率
3.40%
发文量
372
期刊介绍: ACS Sensors is a peer-reviewed research journal that focuses on the dissemination of new and original knowledge in the field of sensor science, particularly those that selectively sense chemical or biological species or processes. The journal covers a broad range of topics, including but not limited to biosensors, chemical sensors, gas sensors, intracellular sensors, single molecule sensors, cell chips, and microfluidic devices. It aims to publish articles that address conceptual advances in sensing technology applicable to various types of analytes or application papers that report on the use of existing sensing concepts in new ways or for new analytes.
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