质子调控型电化学离子突触研究进展

doi:10.15541/jim20240424

无机材料学报 ›› 2025, Vol. 40 ›› Issue (3): 256-270.DOI: 10.15541/jim20240424

质子调控型电化学离子突触研究进展

范晓波¹(), 祖梅¹(), 杨向飞², 宋策¹, 陈晨¹, 王子³, 罗文华², 程海峰¹()

1.国防科技大学空天科学学院, 长沙 410073
2.中国工程物理研究院表面物理与化学重点实验室, 绵阳 621700
3.中南大学粉末冶金研究院, 长沙 410083

收稿日期:2024-10-07 修回日期:2024-11-03 出版日期:2025-03-20 网络出版日期:2025-03-12
通讯作者: 程海峰, 研究员. E-mail: chenghf@nudt.edu.cn;
祖梅, 副研究员. E-mail: zumei2003@163.com
作者简介:范晓波(2000-), 男, 博士研究生. E-mail: fanxiaobo18@163.com
基金资助:
国家自然科学基金(52473117);国家自然科学基金(52203022);湖南省自然科学基金(2024JJ2059);湖南省自然科学基金(2022JJ40547)

Research Progress on Proton-regulated Electrochemical Ionic Synapses

FAN Xiaobo¹(), ZU Mei¹(), YANG Xiangfei², SONG Ce¹, CHEN Chen¹, WANG Zi³, LUO Wenhua², CHENG Haifeng¹()

1. College of Aerospace Science and Engineering, National University of Defense Technology, Changsha 410073, China
2. Science and Technology on Surface Physics and Chemistry Laboratory, China Academy of Engineering Physics, Mianyang 621700, China
3. Powder Metallurgy Research Institute, Central South University, Changsha 410083, China

Received:2024-10-07 Revised:2024-11-03 Published:2025-03-20 Online:2025-03-12
Contact: CHENG Haifeng, professor. E-mail: chenghf@nudt.edu.cn;
ZU Mei, associate professor. E-mail: zumei2003@163.com
About author:FAN Xiaobo (2000-), male, PhD candidate. E-mail: fanxiaobo18@163.com
Supported by:
National Natural Science Foundation of China(52473117);National Natural Science Foundation of China(52203022);Natural Science Foundation of Hunan Province(2024JJ2059);Natural Science Foundation of Hunan Province(2022JJ40547)

摘要/Abstract

摘要：

作为神经网络中数量最庞大的组成部分, 新型人工突触器件的研发成为了硬件实现神经形态计算的关键挑战。基于电化学晶体管的三端突触器件能够有效利用电解质层中的离子来调节通道电导, 也被称为电化学离子突触,该器件通过离子在具有氧化还原活性的沟道材料中的电化学掺杂和恢复过程来模拟生物突触特性。在调制沟道材料电导的离子中, 采用质子(H⁺)作为掺杂粒子的电化学离子突触具有能耗更低、运行速度更快和循环寿命更长等优势。本文综述了近年来质子调控型电化学离子突触的研究进展, 归纳了用于质子调控型电化学离子突触沟道层和电解质层的材料体系, 分析了质子调控型电化学离子突触面临的挑战, 并展望了其未来的发展。

关键词: 神经形态器件, 人工突触, 电化学晶体管, 质子, 综述

Abstract:

Development of novel artificial synaptic devices, which make up the majority of neural networks, has emerged as a pivotal path to hardware realization of neuromorphic computing. An electrochemical ion synapse, also known as a three-terminal synaptic device based on electrochemical transistors, is a device that may efficiently use ions in the electrolyte layer to modify channel conductivity. By electrochemical doping and recovering ions in channel materials exhibiting redox activity, this device mimics biological synaptic properties. The advantages of the electrochemical ion synapse, which uses proton (H⁺) as the doping particle, are lower energy consumption, faster operation, and a longer cycle life among the ions that alter the channel material's conductance. This article reviews the recent research progress on proton-regulated electrochemical ion synapses, summarizes the material systems used for the channel layer and electrolyte layer of proton-regulated electrochemical ion synapses, analyzes the challenges faced by proton-regulated electrochemical ion synapses, and points out directions on their future development.

Key words: neuromorphic device, artificial synapse, electrochemical transistor, proton, review

中图分类号:

TQ174

范晓波, 祖梅, 杨向飞, 宋策, 陈晨, 王子, 罗文华, 程海峰. 质子调控型电化学离子突触研究进展[J]. 无机材料学报, 2025, 40(3): 256-270.

FAN Xiaobo, ZU Mei, YANG Xiangfei, SONG Ce, CHEN Chen, WANG Zi, LUO Wenhua, CHENG Haifeng. Research Progress on Proton-regulated Electrochemical Ionic Synapses[J]. Journal of Inorganic Materials, 2025, 40(3): 256-270.

图/表 8

图1 用于质子调控型电化学离子突触的沟道材料及电解质材料的分类

Fig. 1 Classification of channel materials and electrolyte materials for proton-regulated electrochemical ion synapses

图2 电化学离子突触结构及工作机制示意图[3]

Fig. 2 Device structure and operation principle of an electrochemical ionic synapse[3] (a) Schematic illustration of the device; (b) Schematic illustration of the writing process for an electrochemical ionic synapse based on cation (Mn+) transport and intercalation of M into the channel

表1 不同离子调控型电化学离子突触性能比较[4,6,8 -9,11⇓⇓ -14]

Table 1 Comparison of performance of electrochemical ion synapses regulated by different ions[4,6,8 -9,11⇓⇓ -14]

Action ion	Material (channel/electrolyte)	Dynamic range	Operation voltage/current (pulse width)	Energy consumption	Channel dimension	Ref.
Li⁺	Li_1-_xCoO₂/LiPON	4.5-270 μS	70 mV (2 s)	<10 aJ per write (projection)	L=2 μm	[4]
Li⁺	WO_2.7/Li₃PO₄	0.5-3.5 μS	+3 V (1 s)/-2 V (0.5 s) -2.5 V (1 s)/+1 V (0.5 s)	-	W=5 μm L=5 μm	[6]
O^2-	TiO_2-_x/YSZ (work at 160 ℃)	100-450 nS	±1.5 V (2 μs)	8.1 nJ/mm²	W=250 μm L=8000 μm	[8]
O^2-	WO₃/HfO₂	1.5-3.5 μS	±4 V (10 μs)	1 fJ/(nm²×nS) (projection)	W=20 μm L=80 μm	[9]
H⁺	P(g2T-TT)/ EMIM:TFSI+PVDF-HFP	30-75 μS	±1 V (20 ns)	80 fJ per write	W=15 μm L=45 μm	[11]
	WO₃/PSG	87.6-4.28 MΩ	±10 V (5 ns)/-8.5 V (5 ns)	10 fJ per write	W=50 nm L=150 nm	[12]
	Graphene/Nafion	1.0-2.8 mS	±10 μA (1 ms)	50 aJ/μm²	W=4 mm L=3-5 mm	[13]
	Ti₃C₂T_x/PVA-H₂SO₄	1.6-2.8 mS	±1 V (4 μs)	80 fJ/μm²	W=1000 μm L=20 μm	[14]

图3 有机半导体沟道材料的研究工作[10-11]

Fig. 3 Researches on organic semiconductor channel materials[10-11] (a) A positive Vpre drives protons into the postsynaptic electrode, which results in the compensation of some PSS by the protonated PEI and the reaction is reversed upon applying a negative Vpre[10]; (b) Schematic explaining the decoupling of the read and write operations[10]; (c) Chemical structures of the channel/gate and electrolyte materials[11]; Cycling of device with PEDOT:PSS (d) and p(g2T-TT) (e) as the channel material[11]. Colorful figures are available on website

图4 基于金属氧化物沟道材料的研究工作[12,22,27,29]

Fig. 4 Researches based on metal oxide channel materials[12,22,27,29] (a) Schematic diagram of synaptic transistor modulation based on VO2 channel material[22]; (b) Calculated electronic structure with protonation in WO3[27]; (c) Electronic conductivity and open circuit voltage changed with hydrogen content in WO3, as well as schematic diagram of the device structure[27]; (d) Ultrafast and energy-efficient modulation characteristics of synaptic transistor (channel, WO3;electrolyte, PSG)[12]; (e) Schematic diagram of device structure and STEM micrograph[29]; (f) Endurance test for 108 write-read pulse cycles[29]. Colorful figures are available on website

图5 基于二维沟道材料的研究工作[13-14,34,40 -41]

Fig. 5 Researches based on two-dimensional channel materials[13-14,34,40 -41] (a) Schematic diagram of graphene-based artificial synaptic and conductance per pulse number (20 negative and 20 positive pulses)[13]; (b) Raman spectra of hydrogenated graphene at varied VDS in a switching cycle[34]; (c) Raman mappings of the D peak intensity during VDS sweeps from 0 to 2.5 V and a return to -0.8 V[34]; (d) Schematic representation of hydrogenation reactions between graphene lattice and H+ ions[34]; (e) Schematic diagram of synaptic device based on 2D Ti3C2Tx MXene[14]; (f) MXene channel-based synaptic device resilience to high temperature[14]; (g) Schematic diagram of 2D MXene electrochemical transistor[40]; (h) Schematic diagram of the quasi-2D α-MoO3-based three-terminal synaptic device[41]; (i) Gradual channel current modulation under repeated positive and negative gate voltage pulses[41]. Colorful figures are available on website

图6 离子液体、离子凝胶电解质相关研究[28,46,49 -50]

Fig. 6 Related researches on ionic liquid and ion gel electrolytes[28,46,49 -50] (a) Schematic diagram of a synaptic device using the ionic liquid electrolyte[28]; (b) Contaminated water in ionic liquid could dissociate into H+ and OH−, then the small protons can intercalate into WO3 film to form a HxWO3 phase[28]; (c) FT-IR spectra of double-layered pectin/chitosan composite electrolyte film[46]; (d) FT-IR characterization of sodium alginate thin films[49]; (e) Pictures of konjac tuber and solution, and molecular structure of KGM[50]; (f) AFM image of the prepared KGM film[50]. Colorful figures are available on website

图7 无机固态电解质相关研究[29-30,56⇓ -58]

Fig. 7 Related researches on inorganic solid electrolytes[29-30,56⇓ -58] (a) Schematic diagram of a synaptic device using SiO2 electrolyte[56]; (b) AFM image of PSG thin film surface deposited on Si surface[30]; (c) FT-IR spectra of SiO2 and PSG[30]; (d) SIMS depth profiles for W (black), Zr (blue) and H (red) across device gate stack[29]; (e) Schematic diagram of the change of conductivity of graphene oxide film with water content and its microstructure at a specific water content[57]; (f) Transport of H+ ion through the weak electron cloud of a hexagonal B-N ring of hBN[58]. Colorful figures are available on website

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质子调控型电化学离子突触研究进展

Research Progress on Proton-regulated Electrochemical Ionic Synapses

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