铜锌锡硫硒薄膜太阳能电池一价金属替位的研究进展

doi:10.6023/A20100457

化学学报 ›› 2021, Vol. 79 ›› Issue (3): 303-318.DOI: 10.6023/A20100457 上一篇下一篇

综述

铜锌锡硫硒薄膜太阳能电池一价金属替位的研究进展

周家正^a^,^c, 徐啸^a^,^c, 段碧雯^a^,^c, 石将建^a, 罗艳红^a^,^c^,^d, 吴会觉^a, 李冬梅^a^,^c^,^d^,^*(), 孟庆波^a^,^b^,^c^,^d^,^*()

a 中国科学院物理研究所中国科学院清洁能源前沿研究重点实验室北京市新能源材料与器件重点实验室北京 100190
b 中国科学院大学材料光电研究中心北京 100049
c 中国科学院大学物理科学学院北京 100049
d 松山湖材料实验室广东东莞 523808

投稿日期:2020-10-04 发布日期:2020-12-31
通讯作者: 李冬梅, 孟庆波

作者简介:

周家正, 本科毕业于中南大学能源学院, 现为中国科学院物理研究所博士研究生, 导师为孟庆波研究员和李冬梅研究员, 研究方向是基于湿化学法制备铜锌锡硫硒太阳能电池及其性能研究.

徐啸, 本科毕业于浙江工业大学理学院, 现为中国科学院物理研究所博士研究生, 导师为孟庆波研究员和罗艳红研究员. 研究方向为高效率铜锌锡硫硒太阳能电池.

段碧雯, 本科毕业于华中科技大学化学与化工学院, 现为中国科学院物理研究所博士研究生, 导师为孟庆波研究员. 研究方向高效率锌黄锡矿太阳能电池.

石将建, 现任中国科学院物理研究所副研究员, 2017年中国科学院物理研究所获得博士学位. 研究方向为新型薄膜太阳能电池载流子动力学、界面电荷转移和表面改性研究.

罗艳红, 现任中国科学院物理研究所研究员, 2003年中国科学院化学研究所获得博士学位, 2003~2005年在日本物质科学研究所(NIMS)担任特聘研究员. 研究方向为锌黄锡矿太阳能电池和钙钛矿太阳能电池.

吴会觉, 现任中国科学院物理研究所清洁能源重点实验室高级工程师, 2011年中国科学院理化技术研究所获得博士学位, 研究方向为铜锌锡硫硒太阳能电池和钙钛矿太阳能电池.

李冬梅, 现任中国科学院物理研究所研究员, 1999年吉林大学化学学院获得博士学位, 2000~2003年在日本大学和英国Cardiff大学博士后, 研究方向是新型薄膜太阳能材料与器件, 包括铜锌锡硫硒和钙钛矿太阳能电池及光分解水制氢.

孟庆波, 现任中国科学院物理研究所研究员, 1997年中国科学院长春应化所获得博士学位, 1997~2002年先后在中科院物理所博士后、日本科技厅特别研究员、东京大学和日本神奈川科学技术研究院专任研究员. 2001年入选中科院“引进人才计划”, 2005年获得中科院“引进人才计划”优秀奖, 2007年获得基金委“杰出青年基金”资助, 2013年入选科技北京“百名领军人才”, 2014年基金委创新群体学术带头人. 研究方向是太阳能材料和技术, 包括新型薄膜太阳能电池材料和器件的制备及性能研究、光催化材料的制备与性能研究等.

* E-mail: dmli@iphy.ac.cn;

* E-mail: qbmeng@iphy.ac.cn; Tel.: 0086-010-82649242; Fax: 0086-010-82649242

基金资助:
项目受国家自然科学基金(51961165108); 项目受国家自然科学基金(51421002); 项目受国家自然科学基金(51972332); 项目受国家自然科学基金(51627803); 项目受国家自然科学基金(U2002216)

Research Progress of Metal(I) Substitution in Cu₂ZnSn(S,Se)₄ Thin Film Solar Cells

Jiazheng Zhou^a^,^c, Xiao Xu^a^,^c, Biwen Duan^a^,^c, Jiangjian Shi^a, Yanhong Luo^a^,^c^,^d, Huijue Wu^a, Dongmei Li^a^,^c^,^d^,^*(), Qingbo Meng^a^,^b^,^c^,^d^,^*()

a Key Laboratory for Renewable Energy (CAS), Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences (CAS), Beijing 100190
b Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049
c School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049
d Songshan Lake Materials Laboratory, Dongguan 523808, Guangdong Province

Received:2020-10-04 Published:2020-12-31
Contact: Dongmei Li, Qingbo Meng
Supported by:
National Natural Science Foundation of China (NSFC)(51961165108); National Natural Science Foundation of China (NSFC)(51421002); National Natural Science Foundation of China (NSFC)(51972332); National Natural Science Foundation of China (NSFC)(51627803); National Natural Science Foundation of China (NSFC)(U2002216)

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摘要/Abstract

铜锌锡硫硒(CZTSSe)电池具有组成元素丰度高且环境友好、光吸收系数高、带隙可调、高稳定性等优点, 是一类非常有发展前景的新型薄膜太阳能电池. 目前, CZTSSe电池最高认证效率为12.6%, 与商品化铜铟镓硒(CIGS)电池相比仍然有较大差距, 特别是开路电压(V_OC)和填充因子(FF)偏低. 开压损耗是制约CZTSSe器件效率进一步提升的关键因素之一. 其中, 吸收层带尾态和深能级缺陷及界面能级不匹配是开压损耗大的主因, 而Cu-Zn无序引起的铜锌替位(Cu_Zn)与锌锡替位(Sn_Zn)缺陷又是影响带尾态的关键因素, 因此, 减少Cu_Zn和Sn_Zn缺陷有助于提升V_OC. 一价金属替位能有效改善带尾态、构建合适能带结构, 在一定程度上解决器件开压损耗问题. 但是, 有关一价金属替位如何影响CZTSSe电池性能, 仍然缺乏全面系统的概述. 本文综述了基于一价金属替位方法CZTSSe电池的研究进展. 首先介绍CZTSSe电池的发展历程、工作原理、制备工艺和关键材料等; 其次, 详细讨论一价金属替位的理论研究; 再次, 结合实验进展, 重点讨论一价金属部分替位及完全替位CZTSSe材料的制备及其对带尾态、界面缺陷和能带结构研究; 最后, 对一价金属替位研究的关键科学问题、未来发展潜力等进行讨论和展望, 并提出可能的解决思路.

关键词: 铜锌锡硫硒, Cu_Zn反位缺陷, 一价金属替位, 晶体生长, 带尾态

Cu₂ZnSn(S,Se)₄ solar cell (CZTSSe), as a new type of inorganic thin-film solar cells, has been widely studied in recent years due to the advantages of earth-abundant and environmental-friendly composition elements, high light absorption coefficient and adjustable band gap. CZTSSe solar cell is thus a highly competitive photovoltaic device with potential applications in flexibility, building integrated photovoltaics (BIPV) and so on. So far, 12.6% certified efficiency has been achieved for this kind of solar cells. Open-circuit voltage (V_OC) deficit is always the key factor to unsatisfied efficiency of CZTSSe solar cells, and band tailing, mismatch of energy band structure and deep level defects are the main causes to V_OC deficit. Typically, Cu-Zn disorder-induced defects widely exist in the bulk absorber, due to similar radius of Cu and Zn elements could lead to relatively low formation energy of Cu_Zn and Zn_Cu anti-site defects. Metal(I) substitution is an effective way to solve Cu-Zn disorder, which can well reduce V_OC deficit via lowering band tailing and improving the device structure, leading to better cell performance. However, very few review papers have focused on the metal(I) substitution work. In this review, we will summarize the research progress of metal(I) substitution in Cu₂ZnSn(S,Se)₄ thin film solar cells. Part I introduces the structure and problems of CZTSSe solar cells. Part II shows the origin of metal(I) substitution and theoretical research on substituted materials. Part III focuses on synthetic methods about metal(I) partial substitution devices and influence on crystal growth, band tailing, interface defects and band structure. Part IV briefly introduces metal(I) total substitution devices. Part V anticipates the prospects and bottleneck of metal(I) substitution devices, and give some possible solutions to these current issues.

Key words: Cu₂ZnSn(S,Se)₄, Cu_Zn anti-site defects, metal(I) substitution, crystal growth, band tailing

引用此文

周家正, 徐啸, 段碧雯, 石将建, 罗艳红, 吴会觉, 李冬梅, 孟庆波. 铜锌锡硫硒薄膜太阳能电池一价金属替位的研究进展[J]. 化学学报, 2021, 79(3): 303-318.

Jiazheng Zhou, Xiao Xu, Biwen Duan, Jiangjian Shi, Yanhong Luo, Huijue Wu, Dongmei Li, Qingbo Meng. Research Progress of Metal(I) Substitution in Cu₂ZnSn(S,Se)₄ Thin Film Solar Cells[J]. Acta Chimica Sinica, 2021, 79(3): 303-318.

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图/表 20

图1. CZTSSe器件结构

Figure 1. Structure of CZTSSe devices

图2. (I) CZTSSe结构示意图[23]; (II) CZTSe材料相图[19]

Figure 2. (I) Structure of CZTSSe[23]; (II) phase diagram of CZTSe[19]

图3. (I) CZTS(Se)晶胞结构; (II) K1构型; (III) K2构型; (IV) K3构型; (V) S构型; (VI) M构型

Figure 3. (I) Cell structure of CZTS(Se); (II) K1 configuration; (III) K2 configuration; (IV) K3 configuration; (V) S configuration; (VI) M configuration

	K2	K3	S	M
CZTS	11	393	44	281
CZTSe	12	349	63	255
AZTS	211	496	324	590
AZTSe	186	445	355	1726

表1. 不同构型形成能相对K1构型的差异(以K1构型为0)

Table 1. Different formation energies of configurations relative to the K1 configuration (let the formation energy of K1 configuration be 0)

	CZTS	CZTSe	AZTS	AZTSe
a/nm	0.5461	0.5744	0.5850	0.6109
c/nm	1.0854	1.1406	1.0886	1.1453
c/2a	0.994	0.993	0.930	0.937
V/nm³	0.32369	0.37632	0.37255	0.42742

表2. CZTS(Se)和AZTS(Se)的晶格参数

Table 2. Lattice parameters of CZTS(Se) and AZTS(Se)

图4. (I) 计算所得CZTS, AZTS和LZTS的能带结构; (II) 计算所得Cu2CdSnS4, Cu2ZnSnS4, Ag2ZnSnS4, CuInSe2, CuGaSe2和CdS的带隙排布[44,68]

Figure 4. (I) Calculated band structure of CZTS, AZTS, and LZTS; (II) calculated band alignment between Cu2CdSnS4, Cu2ZnSnS4, Ag2ZnSnS4, CuInSe2, CuGaSe2, and CdS[44,68]

图5. 漫反射光谱测得的(Cu1-xAgx)ZnSnS4 (CAZTS)和(Cu1-xAgx)ZnSnSe4 (CAZTSe)合金固溶体的带隙值[69]

Figure 5. Band-gap energies of (Cu1-xAgx)ZnSnS4 (CAZTS) and (Cu1-xAgx)ZnSnSe4 (CAZTSe) solid solutions estimated from diffuse reflectance spectra[69]

图6. (I) CZTS中低能缺陷的形成能与沿着APQMNPG稳定区域周围的化学势的关系; (II) AZTS中低能缺陷的形成能与沿着APQMNPG稳定区域周围的化学势的关系[20,44]

Figure 6. (I) The formation energy of low-energy defects in CZTS as a function of the chemical potential along the APQMNPG lines surrounding the stable region; (II) The formation energy of low-energy defects in AZTS as a function of the chemical potential along the APQMNPG lines surrounding the stable region[20,44]

图7. Ag2ZnSnS4带隙中本征点缺陷的跃迁能级[44]

Figure 7. The transition energy levels of intrinsic point defects in the band gap of Ag2ZnSnS4[44]

图8. 高Ag掺杂浓度CZTS结构变化: (I) Zn平面替位; (II) Sn平面替位; (III) Zn+Sn平面替位

Figure 8. High Ag doping levels: (I) Substitution in Zn-plane; (II) Substitution in Sn-plane; (III) Substitution in both Zn-plane and Sn-plane

图9. (I)低Ag掺杂水平和(II)高Ag掺杂水平下CZTS中的各种缺陷形成能与Cu化学势的关系图[71]

Figure 9. Formation energies of various defects in CZTS at (I) a low Ag doping level and (II) a high Ag doping level plotted vs the chemical potential of Cu[71]

图10. (I) CZTS相结构和Li掺杂水平的关系; (II) Li占据Wyckoff图不同位点的形成能与Li掺杂水平的关系(Ag作为对比)[67]

Figure 10. (I) The phase structure of CZTS vs Li doping level; (II) the formation energy of Li occupied at different Wyckoff sites vs Li doping level (compared to Ag)[67]

图11. (I) CAZTS, (II) CAZTSe和(III, IV) CLZTS固溶体的X射线衍射图谱[58,69]

Figure 11. X-ray diffraction patterns of (I) CAZTS, (II) CAZTSe, and (III, IV) CLZTS solid solutions[58,69]

图12. 器件制备的不同工艺阶段Li含量(基于电感耦合等离子体质谱法(ICP-MS))[58]

Figure 12. Li content as measured by inductively coupled plasma mass spectrometry (ICP-MS) at different steps of device processing[58]

制备方法	效率	替位量	开压/mV	开压损耗χ	结晶温度/℃	文献
肼溶液, 旋涂法	12.6%	0	513.4	57.94%	500	^[18]
喷雾热解法	7.1%	2% Ag	670	55.61%	600	^[95]
喷雾热解法	7.1%	5% Ag	343.8	—	530	^[96]
乙二醇甲醚, 旋涂法	7.12%	10% Ag	650	—	580	^[99]
二甲亚砜, 旋涂法	7.12%	16% Ag	373	43.46%	530	^[93]
油胺, 热注入法	7.2%	5% Ag	370	45.07%	500	^[97]
乙二醇甲醚, 旋涂法	7.24%	7% Ag	670	51.32% ^a	600	^[85]
共蒸发法	7.6%	—	428	52.14%	540	^[84]
高温固相法	8%	1% Ag	>590	51.85% ^a	740	^[83]
直流溅射法	8.68%	10% Ag	406	48.36%	550	^[78]
高温固相法	8.73%	1% Ag+20% Cd	664	53.33%	740	^[103]
喷雾热解法	10%	35% Ag	477	52.71%	470	^[94]
共蒸发法	10.2%	10% Ag	422.5	52.43%	590	^[81]
硫醇-胺, 旋涂法	10.36%	3% Ag	448	53.78%	480	^[90]
乙二醇甲醚, 旋涂法	10.8%	5% Ag+25% Cd	650	56.21% ^a	600	^[87]
硫醇-胺, 旋涂法	11.2%	(5-30-5)% Ag	464	56.52% ^b	480	^[91]
二甲亚砜, 旋涂法	12.2%	7% Li	531	58.69%	500	^[58]

表3. 效率大于7%的CZTSSe一价金属替位工作汇总

Table 3. Summary of CZTSSe metal(I) substitution works with efficiency >7%

图13. (I) 0%-CZTSSe和(II) 20%-CAZTSSe的导纳谱分析; (III) 0%-CZTSSe和(IV) 20%-CAZTSSe缺陷谱[94]

Figure 13. Admittance spectroscopy measurement of (I) 0%-CZTSSe and (II) 20%-CAZTSSe; defect spectra of (III) 0%-CZTSSe and (IV) 20%-CAZTSSe[94]

图14. Ag替位器件的(I) DLTS图谱(左), 对应的缺陷激活能(右), (II) Urbach分析和(III) PL峰位分析[81,85,90]

Figure 14. (I) DLTS (left), corresponding defect activation energy (right), (II) Urbach model analysis, and (III) PL peak position analysis of Ag substitution devices[81,85,90]

图15. CZTSSe, 20%-CAZTSSe和35%-CAZTSSe的变温开压曲线, EA是VOC向0 K外推所得[94]

Figure 15. VOC-T measurement of CZTSSe, 20%-CAZTSSe, and 35%-CAZTSSe, EA is obtained from the extrapolation of VOC toward 0 K[94]

图16. 暗态和光照下Ag梯度能带示意图[91]

Figure 16. Schematic diagram of Ag gradient band structure in dark and under illumination[91]

图17. CZTS/AZTS/ZnO异质结器件的能带结构

Figure 17. The band alignment of the CZTS/AZTS/ZnO heterojunction photovoltaic device

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铜锌锡硫硒薄膜太阳能电池一价金属替位的研究进展

Research Progress of Metal(I) Substitution in Cu₂ZnSn(S,Se)₄ Thin Film Solar Cells

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铜锌锡硫硒薄膜太阳能电池一价金属替位的研究进展

Research Progress of Metal(I) Substitution in Cu2ZnSn(S,Se)4 Thin Film Solar Cells

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Research Progress of Metal(I) Substitution in Cu₂ZnSn(S,Se)₄ Thin Film Solar Cells