原位低场核磁共振弛豫法定量监测光催化Cr(Ⅵ)还原反应

doi:10.11938/cjmr20202815

摘要/Abstract

摘要：

本文利用原位低场核磁共振（LF-NMR）技术在真实固液反应环境中对光催化还原Cr（Ⅵ）反应进行了定量研究，并对Ag纳米颗粒负载量不同的Ag担载石墨相氮化碳复合光催化剂（Ag/g-C₃N₄）在可见光照射下催化Cr（Ⅵ）还原为Cr（Ⅲ）的性能进行了研究.研究发现，Ag纳米颗粒负载（负载量分别为1 wt.%、2 wt.%、5 wt.%和10 wt.%）可以有效提高g-C₃N₄的光催化性能；且负载量为5 wt.%时光催化性能最优，为无Ag负载的g-C₃N₄的4倍.此外，本文还通过横向弛豫时间（T₂）定量分析了反应体系中顺磁性Cr（Ⅲ）离子的浓度，证实了采用LF-NMR弛豫法评价光催化Cr（Ⅵ）还原反应性能的可行性.

关键词: 原位低场核磁共振, g-C₃N₄, Ag负载, 光催化, Cr(Ⅵ)还原, 横向弛豫时间(T₂)

Abstract:

In this work, operando low-field nuclear magnetic resonance (LF-NMR) technology was used to quantitatively study the photocatalytic reduction of Cr(Ⅵ) in a real solid-liquid reaction environment. The performance of Ag/g-C₃N₄ photocatalysts with different loadings of Ag for the photocatalytic reduction of aqueous Cr(Ⅵ) to Cr(Ⅲ) under visible-light irradiation was systematically investigated. The results showed that the addition of Ag cocatalysts (Ag loading amount: 1 wt.%, 2 wt.%, 5 wt.%, and 10 wt.%) significantly enhanced the photocatalytic performance of g-C₃N₄ photocatalysts, while the optimal content of Ag loading was 5 wt.%, which was greater than that of pristine g-C₃N₄ by a factor of 4.0. Furthermore, we carried out a quantitative analysis on the concentration of paramagnetic Cr(Ⅲ) ions in solution by using the transverse relaxation time (T₂) values, and proved the viability of employing operando LF-NMR relaxometry for monitoring the photocatalytic Cr(Ⅵ) reduction performance.

Key words: operando LF-NMR, g-C₃N₄, Ag loading, photocatalytic, Cr(Ⅵ) reduction, transverse relaxation time (T₂)

中图分类号:

O482.53

牛星星,白志杰,杨翼,高杨文,王雪璐,姚叶锋. 原位低场核磁共振弛豫法定量监测光催化Cr(Ⅵ)还原反应[J]. 波谱学杂志, 2021, 38(3): 403-413.

Xing-xing NIU,Zhi-jie BAI,Yi YANG,Yang-wen GAO,Xue-lu WANG,Ye-feng YAO. A Quantitative Study of Photocatalytic Reduction of Cr(Ⅵ) by Operando Low-Field NMR Relaxometry[J]. Chinese Journal of Magnetic Resonance, 2021, 38(3): 403-413.

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紫外分光光度法Cr(Ⅲ)体系		紫外分光光度法Cr(Ⅵ)-Cr(Ⅲ)混合体系		LF-NMR法Cr(Ⅲ)体系		LF-NMR法Cr(Ⅵ)-Cr(Ⅲ)混合体系
Cr(Ⅲ)浓度/(mg/L)	Cr(Ⅲ)-EDTA吸光度	Cr(Ⅵ)-Cr(Ⅲ)浓度/(mg/L)	Cr(Ⅲ)-EDTA吸光度	Cr(Ⅲ)浓度/(mg/L)	T₂/s	Cr(Ⅵ)-Cr(Ⅲ)浓度/(mg/L)	T₂/s
1	0.007	20-0	0	1	1.528	20-0	3.105
5	0.024	15-5	0.021	5	0.623	15-5	0.604
10	0.038	10-10	0.044	10	0.375	10-10	0.363
15	0.056	5-15	0.056	15	0.276	5-15	0.267
20	0.066	0-20	0.066	20	0.216	0-20	0.216

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