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刘亚超(), 谭晓杰, 李旭东, 王瑞, 王慧, 韩璇, 赵青山()
收稿日期:
2024-01-29
修回日期:
2024-05-20
出版日期:
2024-05-23
通讯作者:
赵青山
作者简介:
刘亚超(1997—),女,硕士研究生,13518629974@163.com
基金资助:
yachao LIU(), xiaojie TAN, xudong LI, rui WANG, hui WANG, xuan HAN, qingshan ZHAO()
Received:
2024-01-29
Revised:
2024-05-20
Online:
2024-05-23
Contact:
qingshan ZHAO
摘要:
氢能因其热值高、清洁无污染等优势,被认为是实现碳中和最有效的能源载体之一,电解水制氢是实现可持续制氢的有效途径。其中,析氧反应(OER)缓慢动力学过程导致水分解效率低下,迫切需要开发高效、稳定的电催化剂。利用多元醇、尿素与CoCl2•6H2O之间的配位作用形成超分子三元低共熔溶剂(DES)体系,通过一锅溶剂热法构建表面粗糙的二维CoCO3纳米片,用于提升电催化OER效率,并针对醇羟基数量对CoCO3形貌及性能影响进行了探究。研究表明,丙三醇、尿素和CoCl2•6H2O三元DES体系制备的CoCO3-Gly催化剂,呈现更蓬松、更薄、更粗糙的片状结构,具有更加优异的OER性能,电流密度在10 mA cm-2时过电位311 mV,经24 h稳定性测试电流保留率达99 %。
中图分类号:
刘亚超, 谭晓杰, 李旭东, 王瑞, 王慧, 韩璇, 赵青山. DES合成高活性CoCO3纳米片及析氧反应性能研究[J]. 化工学报, DOI: 10.11949/0438-1157.20240125.
yachao LIU, xiaojie TAN, xudong LI, rui WANG, hui WANG, xuan HAN, qingshan ZHAO. Synthesis of efficient cobalt carbonate nanosheets based on DES for oxygen evolution reaction[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240125.
图1 CoCO3(a)、(b); CoCO3-PEG(c)、(d); CoCO3-EG(e)、(f)和CoCO3-Gly(g)、(h)的SEM图
Fig.1 SEM of CoCO3(a), (b); CoCO3-PEG(c), (d); CoCO3-EG(e), (f) and CoCO3-Gly(g), (h)
图2 CoCO3(a),CoCO3-PEG(b),CoCO3-EG(c)和CoCO3-Gly(d)的TEM图; CoCO3(e),CoCO3-PEG(f),CoCO3-EG(g)和CoCO3-Gly(h)的HRTEM图; CoCO3-Gly的EDX元素映射图(i)
Fig.2 TEM of CoCO3(a), CoCO3-PEG (b), CoCO3-EG(c) and CoCO3-Gly(d); HRTEM of CoCO3(e), CoCO3-PEG(f), CoCO3-EG(g) and CoCO3-Gly(h); and EDX overlap and element mapping profiles of CoCO3-Gly(i)
图3 CoCO3,CoCO3-PEG,CoCO3-EG和CoCO3-Gly的XRD表征图(a); EPR光谱图(b)和氮气吸脱附曲线(c)
Fig.3 XRD patterns(a); EPR(b) and N2 adsorption-desorption isothermal(c) curves of CoCO3, CoCO3-PEG, CoCO3-EG and CoCO3-Gly
图4 CoCO3, CoCO3-PEG, CoCO3-EG和CoCO3-Gly的XPS全谱(a); C 1s(b); O 1s(c); Co 2p(d)高分辨率XPS图谱
Fig.4 XPS survey spectra(a); High-resolution XPS C1s spectra(b); O1s spectra(c) and Co2p spectra(d) of CoCO3, CoCO3-PEG, CoCO3-EG and CoCO3-Gly
图5 CoCO3,CoCO3-PEG,CoCO3-EG,CoCO3-Gly和RuO2的OER极化曲线图(a); CoCO3,CoCO3-PEG,CoCO3-EG,CoCO3-Gly和RuO2的Tafel图(b)
Fig.5 OER polarization curves of CoCO3, CoCO3-PEG, CoCO3-EG, CoCO3-Gly and RuO2(a); Tafel plot of CoCO3, CoCO3-PEG, CoCO3-EG, CoCO3-Gly and RuO2(b)
图6 CoCO3(a),CoCO3-PEG(b),CoCO3-EG(c)和CoCO3-Gly(d)的CV扫描图(电压区间1.02~1.22 V,扫描速率分别为20、40、60、80、100、120 mV s-1); CoCO3,CoCO3-PEG,CoCO3-EG,CoCO3-Gly在1.12 V电压处扫描速率与电流密度关系图及相应的双电层电容Cdl值(e); CoCO3,CoCO3-PEG,CoCO3-EG和CoCO3-Gly的电化学阻抗图(f)
Fig.6 Cyclic voltammograms of CoCO3(a), CoCO3-PEG(b), CoCO3-EG(c) and CoCO3-Gly(d) in the region of 1.02~1.22 V vs RHE with different scan rates (20, 40, 60, 80, 100 and 120 mV s-1); capacitive currents against scan rate and corresponding Cdl value of CoCO3, CoCO3-PEG, CoCO3-EG and CoCO3-Gly catalysts at 1.12 V(e); EIS Nyquist plots of CoCO3, CoCO3-PEG, CoCO3-EG and CoCO3-Gly(f)
图7 CoCO3(a), CoCO3-PEG(b), CoCO3-EG(c)和CoCO3-Gly(d)恒定电压测试24 h的计时电流曲线图; CoCO3(e), CoCO3-PEG(f), CoCO3-EG(g)和CoCO3-Gly(h)经过3000次CV扫描前后LSV曲线
Fig.7 Long-time stability test of CoCO3(a), CoCO3-PEG(b), CoCO3-EG(c) and CoCO3-Gly(d) at a constant voltage for 24 h. LSV curves of CoCO3(e), CoCO3-PEG(f), CoCO3-EG(g) and CoCO3-Gly(h) before and after 3000 CV scans
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