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

doi:10.6023/A20100457

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (3): 303-318.DOI: 10.6023/A20100457 Previous Articles Next Articles

Review

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)

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

Cite this article

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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Fig. & Tab. 20

Figure 1. Structure of CZTSSe devices

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

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

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

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

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]

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

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]

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

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

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]

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]

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

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]

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

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

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]

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

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

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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