Study of the enhanced thermoelectric properties of ionic hydrogel materials by 2,5-dihydroxybenzenesulfonate

doi:10.11949/0438-1157.20230474

Abstract

Abstract:

At present, ion conductor thermoelectric materials have made some progress in thermoelectric conversion of low-grade heat sources, but there are still problems such as low thermoelectric conversion efficiency and poor sustainability. This study investigated the effect of 2,5-dihydroxybenzenesulfonate (HQS) on the thermoelectric properties of ionic thermoelectric hydrogels under different conditions. By combining proton-coupled electron transfer (PCET) reaction with the Soret effect of protons with high diffusion coefficient, the results showed that the introduction of HQS can enhance the thermoelectric performance with a thermopower of 19.16 mV·K^-1, an ionic thermoelectric figure of merit of 0.98, and a thermoelectric conversion efficiency of 0.19%. At a temperature gradient of 20 K, it can maintain a power output of 120 mW·m^-2 for nearly 2.5 hours.

Key words: ionic thermoelectrics, 2,5-dihydroxybenzenesulfonate, proton-coupled electron transfer, thermoelectric performances

摘要：

目前离子导体热电材料在低品位热源方面的热电转换研究已有一定进展，但仍存在热电转换效率低和可持续性差等问题。研究了2, 5-二羟基苯磺酸盐（HQS）在不同条件下对离子热电水凝胶材料热电性能的影响。利用质子耦合电子转移（PCET）反应协同高扩散系数的质子的Soret效应，结果表明引入HQS可以提升热电性能，其热电势19.16 mV·K^-1，离子热电优值0.98，热电转换效率为0.19%。在20 K温差下，可以维持120 mW·m^-2的功率输出近2.5 h。

关键词: 离子热电, 2, 5-二羟基苯磺酸, 质子耦合电子转移, 热电性能

CLC Number:

TB 34

Yang WANG, Yongqiang DAI, Wei ZENG. Study of the enhanced thermoelectric properties of ionic hydrogel materials by 2,5-dihydroxybenzenesulfonate[J]. CIESC Journal, 2023, 74(9): 3946-3955.

王阳, 戴永强, 曾炜. 2，5-二羟基苯磺酸增强离子水凝胶材料热电性能的研究[J]. 化工学报, 2023, 74(9): 3946-3955.

Figures/Tables 12

Fig.1 Illustration of the redox reactions between HQS and BQS[17]

Fig.2 SEM cross-section images of PAM-co-PAAH hydrogel

Fig.3 Open circuit voltage and thermopower of HQS ionic thermoelectric hydrogel

Fig.4 Transient thermoelectric power variation of HQS ionic thermoelectric hydrogel

Fig.5 The open circuit voltage establishment response of pure acid ion thermoelectric hydrogel and HQS ion thermoelectric hydrogel

Fig.6 AC impedance profiles and conductivity changes of HQS ionic thermoelectric hydrogels with different concentrations and pure acid ionic hydrogels

Fig.7 Ionic thermal conductivity of HQS thermoelectric gel

Fig.8 Cyclic voltammetry curves of HQS hydrogels before and after establishing different temperature gradients

Table 1 Cyclic voltammetry data variation of HQS ionic thermoelectric hydrogels

ΔT/K	V_c/V	I_c/mA	V_a/V	I_a/mA	\|V_c/V_a\|	\|I_c/I_a\|
5	-0.38	-3.32	0.42	3.02	0.90	1.10
10	-0.44	-4.52	0.45	4.22	0.98	1.07
15	-0.46	-6.46	0.46	6.68	1.00	0.97
20	-0.41	-7.06	0.42	7.92	0.98	0.89
25	-0.37	-6.63	0.39	7.63	0.95	0.87
30	-0.35	-5.72	0.38	7.07	0.92	0.81

Fig.9 Performance of load output after voltage establishment of HQS hydrogel

Fig.10 Thermoelectric conversion capacity of HQS hydrogel

Fig.11 Comparison of thermoelectric potential and power density of thermoelectric materials

References 30

1	Forman C, Muritala I K, Pardemann R, et al. Estimating the global waste heat potential[J]. Renewable and Sustainable Energy Reviews, 2016, 57: 1568-1579.
2	Quickenden T I, Mua Y. A review of power generation in aqueous thermogalvanic cells[J]. Journal of the Electrochemical Society, 1995, 142(11): 3985-3994.
3	Li T, Zhang X, Lacey S D, et al. Cellulose ionic conductors with high differential thermal voltage for low-grade heat harvesting[J]. Nature Materials, 2019, 18(6): 608-613.
4	Chipman J. The Soret effect[J]. Journal of the American Chemical Society, 1926, 48(10): 2577-2589.
5	Alam H, Ramakrishna S. A review on the enhancement of figure of merit from bulk to nano-thermoelectric materials[J]. Nano Energy, 2013, 2(2): 190-212.
6	Wu X, Gao N W, Jia H Y, et al. Thermoelectric converters based on ionic conductors[J]. Chemistry-An Asian Journal, 2021, 16(2): 129-141.
7	Choi P, Jalani N H, Datta R. Thermodynamics and proton transport in Nafion(Ⅰ): Membrane swelling, sorption, and ion-exchange equilibrium[J]. Journal of the Electrochemical Society, 2005, 152(3): E84-E89.
8	Choi P, Jalani N H, Datta R. Thermodynamics and proton transport in Nafion(Ⅱ): Proton diffusion mechanisms and conductivity[J]. Journal of the Electrochemical Society, 2005, 152(3): E123-E130.
9	Choi P, Jalani N H, Datta R. Thermodynamics and proton transport in Nafion(Ⅲ): Proton transport in Nafion/sulfated ZrO₂ nanocomposite membranes[J]. Journal of the Electrochemical Society, 2005, 152(8): A1548-A1554.
10	Jalani N H, Choi P, Datta R. TEOM: a novel technique for investigating sorption in proton-exchange membranes[J]. Journal of Membrane Science, 2005, 254(1/2): 31-38.
11	Alt H, Binder H, Köhling A, et al. Investigation into the use of quinone compounds-for battery cathodes[J]. Electrochimica Acta, 1972, 17(5): 873-887.
12	Guo B S, Hoshino Y, Gao F, et al. Thermocells driven by phase transition of hydrogel nanoparticles[J]. Journal of the American Chemical Society, 2020, 142(41): 17318-17322.
13	Chen L B, Bai H, Huang Z F, et al. Mechanism investigation and suppression of self-discharge in active electrolyte enhanced supercapacitors[J]. Energy & Environmental Science, 2014, 7(5): 1750-1759.
14	Deng Q J, Tian C C, Luo Z B, et al. Organic 2,5-dihydroxy-1,4-benzoquinone potassium salt with ultrahigh initial coulombic efficiency for potassium-ion batteries[J]. Chemical Communications, 2020, 56(81): 12234-12237.
15	Frackowiak E, Meller M, Menzel J, et al. Redox-active electrolyte for supercapacitor application[J]. Faraday Discussions, 2014, 172: 179-198.
16	Komura T, Yamaguchi T, Furuta K, et al. Irreversible transformation of polypyrrole-bound viologen with two-electron reduction in acidic aqueous solutions[J]. Journal of Electroanalytical Chemistry, 2002, 534(2): 123-130.
17	Zhang Z J, Chen X Y. Illustrating the effect of electron withdrawing and electron donating groups adherent to p-hydroquinone on supercapacitor performance: the cases of sulfonic acid and methoxyl groups[J]. Electrochimica Acta, 2018, 282: 563-574.
18	Wang Y, Dai Y Q, Li L B, et al. Proton-coupled electron transfer aided thermoelectric energy conversion and storage[J]. Angewandte Chemie International Edition, 2023, 62(35): 202219136.
19	冉广芬, 马海州, 孟瑞英, 等. 四苯硼钠-季铵盐容量法快速测钾[J]. 盐湖研究, 2009, 17(2): 39-42.
	Ran G F, Ma H Z, Meng R Y, et al. Rapid determination of potassium content by sodium tetraphenylboron-quaternary ammonium salt volumetric method[J]. Journal of Salt Lake Research, 2009, 17(2): 39-42.
20	Gao H C, Guo B K, Song J E, et al. A composite gel-polymer/glass-fiber electrolyte for sodium-ion batteries[J]. Advanced Energy Materials, 2015, 5(9): 1402235.
21	Wang H, Hsu J H, Yi S I, et al. Thermally driven large N-type voltage responses from hybrids of carbon nanotubes and poly(3,4-ethylenedioxythiophene) with tetrakis(dimethylamino)ethylene[J]. Advanced Materials, 2015, 27(43): 6855-6861.
22	Kim S L, Lin H T, Yu C. Thermally chargeable solid-state supercapacitor[J]. Advanced Energy Materials, 2016, 6(18): 1600546.
23	Zhao D, Wang H, Khan Z U, et al. Ionic thermoelectric supercapacitors[J]. Energy & Environmental Science, 2016, 9(4): 1450-1457.
24	Li Y C, Li Q K, Zhang X B, et al. 3D hierarchical electrodes boosting ultrahigh power output for gelatin-KCl-FeCN^{4–/ 3–} ionic thermoelectric cells[J]. Advanced Energy Materials, 2022, 12(14): 2103666.
25	Buckingham M A, Marken F, Aldous L. The thermoelectrochemistry of the aqueous iron(ⅱ)/iron(ⅲ) redox couple: significance of the anion and pH in thermogalvanic thermal-to-electrical energy conversion[J]. Sustainable Energy & Fuels, 2018, 2(12): 2717-2726.
26	Wu J, Black J J, Aldous L. Thermoelectrochemistry using conventional and novel gelled electrolytes in heat-to-current thermocells[J]. Electrochimica Acta, 2017, 225: 482-492.
27	Zhao D, Martinelli A, Willfahrt A, et al. Polymer gels with tunable ionic Seebeck coefficient for ultra-sensitive printed thermopiles[J]. Nature Communications, 2019, 10: 1093.
28	Duan J J, Feng G, Yu B Y, et al. Aqueous thermogalvanic cells with a high Seebeck coefficient for low-grade heat harvest[J]. Nature Communications, 2018, 9: 5146.
29	Cheng H L, He X, Fan Z, et al. Flexible quasi-solid state ionogels with remarkable Seebeck coefficient and high thermoelectric properties[J]. Advanced Energy Materials, 2019, 9(32): 1901085.
30	Han C G, Qian X, Li Q K, et al. Giant thermopower of ionic gelatin near room temperature[J]. Science, 2020, 368(6495): 1091-1098.

[1]	Yuanchao LIU, Bin GUAN, Jianbin ZHONG, Yifan XU, Xuhao JIANG, Duan LI. Investigation of thermoelectric transport properties of single-layer XSe₂(X=Zr/Hf) [J]. CIESC Journal, 2023, 74(9): 3968-3978.
[2]	Yuanchao LIU, Xuhao JIANG, Ke SHAO, Yifan XU, Jianbin ZHONG, Zhuan LI. Influence of geometrical dimensions and defects on the thermal transport properties of graphyne nanoribbons [J]. CIESC Journal, 2023, 74(6): 2708-2716.
[3]	Jialin DAI, Weidong BI, Yumei YONG, Wenqiang CHEN, Hanyang MO, Bing SUN, Chao YANG. Effect of thermophysical properties on the heat transfer characteristics of solid-liquid phase change for composite PCMs [J]. CIESC Journal, 2023, 74(5): 1914-1927.
[4]	Xuehong WU, Linlin LUAN, Yanan CHEN, Min ZHAO, Cai LYU, Yong LIU. Preparation and thermal properties of degradable flexible phase change films [J]. CIESC Journal, 2023, 74(4): 1818-1826.
[5]	Chi YIN, Zhengguo ZHANG, Ziye LING, Xiaoming FANG. Combining paraffin@silica nanocapsules with carbon fiber to develop a phase change thermal interface material for efficient heat dissipation [J]. CIESC Journal, 2023, 74(4): 1795-1804.
[6]	Jianxin CHEN, Ruijie ZHU, Nan SHENG, Chunyu ZHU, Zhonghao RAO. Preparation of cellulose-derived biomass porous carbon and its supercapacitor performance [J]. CIESC Journal, 2022, 73(9): 4194-4206.
[7]	Chuyue CAI, Xiaoming FANG, Zhengguo ZHANG, Ziye LING. Enhancing heat dissipation performance of paraffin/silicone rubber phase change thermal pad by introducing carbon nanotubes [J]. CIESC Journal, 2022, 73(7): 2874-2884.
[8]	Xinbin NIE, Dehao ZHANG, Weicheng YAN. Research progress of functional microbubble materials [J]. CIESC Journal, 2021, 72(8): 3984-3996.
[9]	HAN Xiao,CHEN Yuting,SU Baogen,BAO Zongbi,ZHANG Zhiguo,YANG Yiwen,REN Qilong,YANG Qiwei. Advances in adsorbents for hexane isomers separation [J]. CIESC Journal, 2021, 72(7): 3445-3465.
[10]	MA Jiazhuang, CHEN Ying, LI Kaitao, LIN Yanjun. Research progress on magnesium-based intercalated functional materials [J]. CIESC Journal, 2021, 72(6): 2922-2933.
[11]	GAO Wa, RAN Xiangkun, ZHAO Hanqing, ZHAO Yufei. Research progress of catalytic materials based on Mg-based layered double hydroxides [J]. CIESC Journal, 2021, 72(6): 2934-2956.
[12]	CHEN Rundao, ZHENG Fang, GUO Lidong, YANG Qiwei, ZHANG Zhiguo, YANG Yiwen, REN Qilong, BAO Zongbi. Advancements in adsorption separation of Xe/Kr noble gases [J]. CIESC Journal, 2021, 72(1): 14-26.
[13]	Wei ZHOU, Li CHEN, Jingcheng DU, Luxi TAN, Lichun DONG, Cailong ZHOU. Bio-inspired fog harvesting materials: from fundamental research to promotional strategy [J]. CIESC Journal, 2020, 71(10): 4532-4552.
[14]	Shuang WEN, Xiaojie JU, Rui XIE, Wei WANG, Zhuang LIU, Liangyin CHU. Fabrication and controlled-release properties of intestinal-targeted Ca-alginate-based capsules [J]. CIESC Journal, 2020, 71(8): 3797-3806.
[15]	Yating ZHANG, Bochao ZHANG, Jianlan ZHANG, Keke LI, Yongqiang DANG, Yingfeng DUAN. Research progress in “bottom-up” chemical synthesis of nanographenes [J]. CIESC Journal, 2020, 71(6): 2628-2642.