NaCu5S3复合NixFe-LDH的结构对水解氧析出性能的影响

白成; 吴用; 辛雨慈; 牟俊峰; 江俊颖; 丁鼎; 夏雷; 余鹏

doi:10.7498/aps.72.20230146

摘要

析氧反应 (OER) 在锌空气电池、燃料电池和电解水等能源储存和转换设备中都有至关重要的作用. 然而OER过程涉及四电子转移, 导致反应动力学缓慢. 尽管贵金属氧化物被认为是最先进的OER电催化剂, 但昂贵的价格以及稀缺性限制了其商业应用. 因此, 本工作结合水热和水浴法制备了NaCu₅S₃@Ni_xFe-LDH (x = 1, 2, 3, 4) 纳米片阵列复合电催化剂. 对样品的结构进行了表征, 结果显示NaCu₅S₃和Ni₂Fe-LDH充分混合, 形成紧密结合的界面, 有利于电荷的快速转移, 这将增强两相界面处的电子调控作用, 改变其局域结构特性, 促进OER电催化性能. 电化学测试结果显示, 当电流密度为20 mA·cm^–2时, NaCu₅S₃@Ni₂Fe-LDH在1.0 M KOH电解液中的氧析出过电位仅为227 mV, 电催化性能优于原始的NaCu₅S₃ (271 mV) 和Ni₂Fe-LDH (275 mV), 并且具有长达72 h的稳定性. 此外, NaCu₅S₃@Ni₂Fe-LDH复合电催化剂具有较小的电荷转移电阻, 较大的双层电容值 (10.0 mF·cm^–2) 和电化学活性表面积 (250 cm²), 有利于OER的进行. 本工作为设计廉价、高效且稳定的OER复合电催化剂提供了切实可行的实践路径.

关键词:

Abstract

The oxygen evolution reaction (OER) plays a critical role in energy storage and conversion devices such as zinc-air batteries, fuel cells, and electrolysis water. However, the OER process involves a four-electron transfer, leading to slow reaction kinetics. Therefore, it is necessary to explore an efficient, inexpensive, and durable electrocatalysts to accelerate the OER process. Noble metal oxides are considered the most advanced OER electrocatalysts, but their high price and scarcity limit their commercial applications. Thus, researchers have started exploring other low-cost materials as alternatives. Nanocomposite materials have emerged as a promising alternative to expensive and scarce noble metal oxide electrocatalysts for OER. Therefore, this work synthesizes novel nanocomposite materials, NaCu₅S₃@Ni_xFe-LDH (x = 1, 2, 3, 4) nanosheet array via hydrothermal and water bath methods. The structure and morphology of each product are characterized, indicating a tightly integrated interface between NaCu₅S₃ and Ni₂Fe-LDH, which facilitates rapid charge transfer and enhancement of electron regulation at the interface. This changes the local structure characteristics and promotes the OER catalytic performance. Electrochemical characterization results show that in a 1.0 M KOH electrolyte, the overpotential of NaCu₅S₃@Ni₂Fe-LDH for OER at a current density of 20 mA/cm² is only 227 mV, significantly lower than that of the original NaCu₅S₃ (271 mV) and Ni₂Fe-LDH (275 mV), with stability duration reaching 72 h. Electrochemical results also reveal that with the increase of overpotential, NaCu₅S₃@Ni₂Fe-LDH shows a significant oxidation peak between 1.35–1.45 (V vs. RHE), which leads to the activation of Ni²⁺ to Ni³⁺ high oxidation state. The high oxidation state of Ni will promote the OER. The NaCu₅S₃@Ni₂Fe-LDH composite electrocatalyst exhibits lower charge transfer resistance, higher double layer capacitance value (10.0 mF/cm²), and electrochemical active surface area (250 cm²), which are also beneficial to promoting OER. This study highlights the potential of nanocomposite materials as cost-effective alternatives to noble metal oxide electrocatalysts for OER. The NaCu₅S₃@Ni₂Fe-LDH composite electrocatalyst exhibits excellent OER performance with a low overpotential, high stability, and favorable electrochemical properties. This research provides a valuable insight into the design and development of efficient and sustainable electrocatalysts for energy conversion and storage applications.

Keywords:

作者及机构信息

1.
重庆师范大学物理与电子工程学院, 光电功能材料重庆市重点实验室, 重庆　401331

2.
上海大学材料研究所, 上海　200072

通信作者: 吴用, wy_yp@shu.edu.cn ; 余鹏, pengyu@cqnu.edu.cn

基金项目: 国家自然科学基金 (批准号: 52071043) 和重庆市教委科学技术研究重点项目(批准号: KJZD-K201900501) 资助的课题.

Authors and contacts

1.
Chongqing Key Laboratory of Photo-Electric Functional Materials, College of Physics and Electronic Engineering, Chongqing Normal University, Chongqing 401331, China

2.
Institute of Materials, Shanghai University, Shanghai 200072, China

Corresponding author: Wu Yong, wy_yp@shu.edu.cn ; Yu Peng, pengyu@cqnu.edu.cn

Funds: Project supported by the National Nature Science Foundation of China (Grant No. 52071043) and the Key Science and Technology Research Program Project of the Chongqing Education Commission of China (Grant No. KJZD-K201900501).

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补充材料

10-20230146(补充材料).pdf

参考文献

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施引文献

图 1 NaCu₅S₃, NaCu₅S₃@NiFe-LDH, NaCu₅S₃@Ni₂Fe-LDH, NaCu₅S₃@Ni₃Fe-LDH和NaCu₅S₃@Ni₄Fe-LDH 的XRD衍射谱图

Fig. 1. XRD patterns of the NaCu₅S₃, NaCu₅S₃@NiFe-LDH, NaCu₅S₃@Ni₂Fe-LDH, NaCu₅S₃@Ni₃Fe-LDH and NaCu₅S₃@Ni₄Fe-LDH.

下载: 全尺寸图片幻灯片

图 2 (a)—(e) NaCu₅S₃, NaCu₅S₃@NiFe-LDH, NaCu₅S₃@Ni₂Fe-LDH, NaCu₅S₃@Ni₃Fe-LDH和NaCu₅S₃@Ni₄Fe-LDH的SEM图像; (f)—(i) NaCu₅S₃和NaCu₅S₃@Ni₂Fe-LDH的TEM和HRTEM图像; (j), (k) NaCu₅S₃和NaCu₅S₃@Ni₂Fe-LDH的EDS能谱图

Fig. 2. (a)–(e) SEM image of the NaCu₅S₃, NaCu₅S₃@NiFe-LDH, NaCu₅S₃@Ni₂Fe-LDH, NaCu₅S₃@Ni₃Fe-LDH and NaCu₅S₃@Ni₄Fe-LDH; (f)–(i) TEM and HRTEM images of the NaCu₅S₃ and NaCu₅S₃@Ni₂Fe-LDH; (j), (k) EDS images for the NaCu₅S₃ and NaCu₅S₃@Ni₂Fe-LDH.

下载: 全尺寸图片幻灯片

图 3 (a)—(c) NaCu₅S₃和NaCu₅S₃@Ni₂Fe-LDH Na 1s, Cu 2p和S 2p XPS能谱; (d), (e) NaCu₅S₃@Ni₂Fe-LDH Ni 2p和Fe 2p XPS能谱; (f) NaCu₅S₃和NaCu₅S₃@Ni₂Fe-LDH XPS能谱

Fig. 3. (a)–(c) Na 1s, Cu 2p and S 2p XPS spectra of NaCu₅S₃ and NaCu₅S₃@Ni₂Fe-LDH; (d), (e) Ni 2p and Fe 2p XPS spectra of the NaCu₅S₃@Ni₂Fe-LDH; (f) XPS spectra of NaCu₅S₃ and NaCu₅S₃@Ni₂Fe-LDH.

下载: 全尺寸图片幻灯片

图 4 NaCu₅S₃@NiFe-LDH, NaCu₅S₃@Ni₂Fe-LDH, NaCu₅S₃@Ni₃Fe-LDH, NaCu₅S₃@Ni₄Fe-LDH, NaCu₅S₃和Ni₂Fe-LDH　(a) LSV极化曲线; (b) Tafel斜率; (c) EIS; (d) C_dl; (e) ECSA; (f) NaCu₅S₃@Ni₂Fe-LDH CP曲线

Fig. 4. NaCu₅S₃@NiFe-LDH, NaCu₅S₃@Ni₂Fe-LDH, NaCu₅S₃@Ni₃Fe-LDH, NaCu₅S₃@Ni₄Fe-LDH, NaCu₅S₃ and Ni₂Fe-LDH: (a) LSV polarization curves; (b) Tafel slope; (c) EIS; (d) C_dl; (e) ECSA; (f) CP curve of NaCu₅S₃@Ni₂Fe-LDH.

下载: 全尺寸图片幻灯片

图 5 (a)—(c) NaCu₅S₃ OER前后的Na 1s, Cu 2p和S 2p XPS能谱; (d)—(h) NaCu₅S₃@Ni₂Fe-LDH OER前后的Na 1s, Cu 2p, S 2p, Ni 2p和Fe 2p XPS能谱

Fig. 5. (a)–(c) Na 1s, Cu 2p and S 2p XPS spectra of the NaCu₅S₃ before and after OER; (d)–(h) Na 1s, Cu 2p, S 2p, Ni 2p and Fe 2p XPS spectra of the NaCu₅S₃@Ni₂Fe-LDH before and after OER.

下载: 全尺寸图片幻灯片

表 1 1 M KOH电解液中催化剂的OER活性比较

Table 1. Comparison of OER activity of catalysts in 1 M KOH electrolytes.

Catalyst	Electrolyte	Overpotential/mV	Current density /(mA·cm^–2)	Ref.
NaCu₅S₃@NiFe-LDH	1 M KOH	254	20	This work
NaCu₅S₃@Ni₂Fe-LDH	1 M KOH	227	20	This work
NaCu₅S₃@Ni₃Fe-LDH	1 M KOH	248	20	This work
NaCu₅S₃@Ni₄Fe-LDH	1 M KOH	259	20	This work
NaCu₅S₃	1 M KOH	271	20	This work
Cu₉S₅/NF	1 M KOH	298	10	[33]
CuS-FSM	1 M KOH	408	10	[34]
CoO@Cu₂S	1 M KOH	277	10	[35]
Cu₂S/CF	1 M KOH	336	20	[36]
CuNiS	1 M KOH	337	10	[37]
Cu-NiS₂	1 M KOH	232	10	[25]
Cu₂S/TiO₂/Cu₂S	1 M KOH	284	10	[13]

下载: 导出CSV

map

[1]	Zhang Z H, Wang C L, Ma X L, Liu F, Xiao H, Zhang J, Lin Z, Hao Z P 2021 Small 17 2103785 Google Scholar
[2]	Zhao X H, Pattengale B, Fan D H, Zou Z H, Zhao Y Q, Du J, Huang J E, Xu C L 2018 ACS Energy Lett. 3 2520 Google Scholar
[3]	Zhao X, Zheng X R, Lu Q, Li Y, Xiao F P, Tang B, Wang S X, Yu D Y W, Rogach A L 2023 EcoMat. 5 e12293 Google Scholar
[4]	Song J J, Wei C, Huang Z F, Liu C T, Zeng L, Wang X, Xu Z C 2020 J. Chem. Soc. Rev. 49 2196 Google Scholar
[5]	Gao J J, Xu C Q, Hung S F, Liu W, Cai W Z, Zeng Z P, Jia C M, Chen H M, Xiao H, Li J, Huang Y Q, Liu B 2019 J. Am. Chem. Soc. 141 3014 Google Scholar
[6]	孙涛, 袁健美 2023 72 028901 Google Scholar Sun T, Yuan J M 2023 Acta Phys. Sin. 72 028901 Google Scholar
[7]	汤衍浩 2023 72 027802 Google Scholar Tang Y H 2023 Acta Phys. Sin. 72 027802 Google Scholar
[8]	She Z W, Kibsgaard J, Dickens C F, Chorkendorff I B, Norskov J K, Jaramillo T F 2017 Science 355 4998 Google Scholar
[9]	Guo Y N, Park T, Yi J W, Henzie J, Kim J, Wang Z L, Jiang B, Bando Y, Sugahara Y, Tang J, Yamauchi Y 2019 Adv. Mater. 31 1807134 Google Scholar
[10]	Chia X, Eng A Y S, Ambrosi A, Tan S M, Pumera M 2015 Chem. Rev. 115 11941 Google Scholar
[11]	Zheng Y, Jiao Y, Jaroniec M, Qiao S Z 2015 Angew. Chem. Int. Ed. 54 52 Google Scholar
[12]	李雨芃, 汤秀章, 陈欣南, 高春宇, 陈雁南, 范澄军, 吕建友 2023 72 029501 Google Scholar Li Y P, Tang X Z, Chen X N, Gao C Y, Chen Y N, Fan C J, Lü J Y 2023 Acta Phys. Sin. 72 029501 Google Scholar
[13]	Deng S J, Shen Y B, Xie D, Lu Y F, Yu X L, Yang L, Wang X L, Xia X H, Tu J P 2019 J. Energy Chem. 39 61 Google Scholar
[14]	Liu G M, Schulmeyer T, Brötz J, Klein A, Jaegermann W 2003 Thin Solid Films 431 477 Google Scholar
[15]	邓晨华, 于忠海, 王宇涛, 孔森, 周超, 杨森 2023 72 027501 Google Scholar Deng C H, Yu Z H, Wang Y T, Kong S, Zhou C, Yang S 2023 Acta Phys. Sin. 72 027501 Google Scholar
[16]	Zhao J, Zhang J J, Li Z Y, Bu X H 2020 Small 16 2003916 Google Scholar
[17]	Lü L, Yang Z X, Chen K, Wang C D, Xiong Y J 2019 Adv. Energy Mater. 9 1803358 Google Scholar
[18]	Huang Z N, Liao X P, Zhang W B, Hu J L, Gao Q S 2022 ACS Catal. 12 13951 Google Scholar
[19]	Lin X J, Cao S F, Chen H Y, Chen X D, Wang Z J, Zhou S N, Xu H, Liu S Y, Wei S X, Lu X Q 2022 Chem. Engine. J. 433 133524 Google Scholar
[20]	Song S Z, Mu L H, Jiang Y, Sun J, Zhang Y, Shi G S, Sun H N 2022 ACS Appl. Mater. Inter. 14 47560 Google Scholar
[21]	Li D, Qin Y Y, Liu J, Zhao H Y, Sun Z J, Chen G B, Wu D Y, Su Y Q, Ding S J, Xiao C H V 2022 Adv. Funct. Mater. 32 2107056 Google Scholar
[22]	Lv L, He X B, Wang J S, Ruan Y J, Yang S X, Yuan H, Zhang T R 2021 Appl. Catal. B 298 120531 Google Scholar
[23]	Gu Z X, Yang N, Han P, Kuang M, Mei B B, Jiang Z, Zhong J, Li L, Zheng G F 2019 Small Methods 3 1800449 Google Scholar
[24]	Du C F, Dinh K N, Liang Q H, Zheng Y, Luo Y B, Zhang J L, Yan Q Y 2018 Adv. Energy Mater. 8 1801127 Google Scholar
[25]	Dinh K N, Sun Y X, Pei Z X, Yuan Z W, Suwardi A, Huang Q W, Liao X Z, Wang Z G, Chen Y, Yan Q Y 2020 Small 16 1905885 Google Scholar
[26]	Liu M J, Min K A, Han B C, Lee L Y S 2021 Adv. Energy Mater. 11 2101281 Google Scholar
[27]	Li A, Zhang Z, Feng J, Lü F, Li Y, Wang R, Lu M, Gupta R B, Xi P, Zhang S 2018 J. Am. Chem. Soc. 140 17624 Google Scholar
[28]	Xie Q X, Ren D, Bai L C, Ge R L, Zhou W H, Bai L, Xie W, Wang J H, Grätzel M, Luo J S 2023 Chin. J. Catalysis 44 127 Google Scholar
[29]	Li S, Chen B B, Wang Y, Ye M Y, Aken P A V, Cheng C, Thomas A 2021 Nat. Mater. 20 1240 Google Scholar
[30]	Wan K, Luo J S, Zhou C, Zhang T, Arbiol J, Lu X H, Mao B W, Zhang X, Fransaer J 2019 Adv. Funct. Mater. 29 1900315 Google Scholar
[31]	Bai Y K, Wu Y, Zhou X C, Ye Y F, Nie K Q, Wang J, Xie M, Zhang Z X, Liu Z J, Cheng T, Gao C B 2022 Nat. Commun. 13 6094 Google Scholar
[32]	Zhu J L, Qian J M, Peng X B, Xia B R, Gao D Q 2023 Nano-Micro Lett. 15 30 Google Scholar
[33]	Chakraborty B, Kalra S, Beltrán-Suito R, Das C, Hellmann T, Menezes W P, Driess M 2020 Chem. Asian J. 15 852 Google Scholar
[34]	Liang H J, Shuang W, Zhang Y T, Chao S J, Han H J, Wang X B, Zhang H, Yang L 2018 Chem. Electro. Chem. 5 494 Google Scholar
[35]	Li Y M, Zhang X Y, Zhuo S Y, Liu S L, Han A X, Li L G, Tian Y 2021 Appl. Surf. Sci. 555 149441 Google Scholar
[36]	He L B, Zhou D, Lin Y, Ge R X, Hou X D, Sun X P, Zheng C B 2018 ACS Catal. 8 3859 Google Scholar
[37]	Chinnadurai D, Rajendiran R, Kandasamy P 2022 J. Colloid Inter. Sci. 606 101 Google Scholar
[38]	Tan L, Yu J T, Wang C, Wang H F, Liu X, Gao H T, Xin L T, Liu D Z, Hou W G, Zhan T R 2022 Adv. Funct. Mater. 32 2200951
[39]	Sun S, Zhou X, Cong B, Hong W, Chen G 2020 ACS Catal. 10 9086 Google Scholar
[40]	Zhang J, Wang T, Pohl D, Rellinghaus B, Dong R H, Liu S H, Zhuang X D, Feng X L 2016 Angew. Chem. Int. Ed. 55 6702 Google Scholar
[41]	Zhao Z L, Wu H X, He H L, Xu X L, Jin Y D 2014 Adv. Funct. Mater. 24 4698 Google Scholar
[42]	Li Y, Chen G, Zhu Y, Hu Z, Chan T, She S, Dai J, Zhou W, Shao Z 2021 Adv. Funct. Mater. 31 2103569 Google Scholar

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NaCu₅S₃复合Ni_xFe-LDH的结构对水解氧析出性能的影响

Effect of NaCu₅S₃ composite Ni_xFe-LDH structure on hydrolysis oxygen evolution performance

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Abstract

作者及机构信息

1.
重庆师范大学物理与电子工程学院, 光电功能材料重庆市重点实验室, 重庆　401331

2.
上海大学材料研究所, 上海　200072

通信作者: 吴用, wy_yp@shu.edu.cn ; 余鹏, pengyu@cqnu.edu.cn

Authors and contacts

1.
Chongqing Key Laboratory of Photo-Electric Functional Materials, College of Physics and Electronic Engineering, Chongqing Normal University, Chongqing 401331, China

2.
Institute of Materials, Shanghai University, Shanghai 200072, China

Corresponding author: Wu Yong, wy_yp@shu.edu.cn ; Yu Peng, pengyu@cqnu.edu.cn

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