Research progress of passivation layer technology for crystalline silicon solar cells

YUAN Heze; CHEN Xinliang; LIANG Bingquan; SUN Aixin; WANG Xuejiao; ZHAO Ying; ZHANG Xiaodan

doi:10.7498/aps.74.20241292

Abstract

With the rapid development of photovoltaic technology, crystalline silicon (c-Si) solar cells, as the mainstream photovoltaic devices, have received significant attention due to their excellent performances. In particular, silicon heterojunction (SHJ) solar cells, tunnel oxide passivated contact (TOPCon), and passivated emitter and rear cell (PERC) represent the cutting-edge technologies in c-Si solar cells. The surface passivation layer of crystalline silicon solar cells, as one of the key factors to improve cell performances, has been closely linked to the development of crystalline silicon solar cells. Due to the complex mechanism of passivation layer and the high requirements of experimental research, achieving high quality surface passivation is challenging. In this paper, the key issues and research progress of interface passivation technologies for SHJ, TOPCon, and PERC solar cells are comprehensively reviewed. Firstly, the research progress of key technological breakthrough in SHJ solar cell is reviewed systematically, and the influences of growth conditions and doping layer on the passivation performances of SHJ solar cell are discussed in detail. Secondly, the important strategies and research achievements for improving the passivation performances of TOPCon and PERC solar cells in the past five years are systematically described. Finally, the development trend of passivation layer technology is prospected. This review provides valuable insights for improving future technology and enhancing performance of c-Si solar cells.

Keywords:

Authors and contacts

State Key Laboratory of Photovoltaic Materials and Cells, Tianjin Key Laboratory of Efficient Utilization of Solar Energy, Institute of Optoelectronic Thin Film Devices and Technology, Nankai University, Tianjin 300350

Corresponding author: CHEN Xinliang, cxlruzhou@163.com

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2022YFB4200102) and the Natural Science Foundation of Tianjin, China (Grant No. 21JCYBJC00270).

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图 1 (a), (b) PERC太阳电池结构^[7]和制造流程图^[6]; (c), (d) TOPCon太阳电池结构和制造流程图^[9]; (e), (f) SHJ太阳电池结构图和制造流程图^[16]

Figure 1. (a), (b) PERC solar cell structure^[7] and manufacturing process diagram^[6]; (c), (d) TOPCon solar cell structure and manufacturing process diagram^[9]; (e), (f) SHJ solar cell structure diagram and manufacturing process diagram^[16].

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图 2 (a) c-Si材料原子结构示意图, $ \left\langle{110}\right\rangle $晶向^[24]; (b) a-Si材料原子结构示意图^[24]; (c) a-Si:H材料原子结构示意图^[24]; (d) a-Si:H钝化c-Si结构示意图

Figure 2. (a) Schematic diagram of c-Si material atomic structure, $ \left\langle{110}\right\rangle $ crystal orientation^[24]; (b) schematic diagram of a-Si material atomic structure^[24]; (c) schematic diagram of a-Si:H material atomic structure^[24]; (d) schematic diagram of a-Si:H passivated c-Si structure.

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图 3 (a) 薄膜的R^*和C_H随氢稀释比R_H ($ {R_{\text{H}}} = {{{f_{{{\text{H}}_2}}}} {/} {{f_{{\text{Si}}{{\text{H}}_4}}}}} $)的变化, 灰色区域是非晶-微晶过渡区^[27]; (b) HPT前后的过渡区的i-a-Si:H与c-Si(n)的交界面的HR-TEM图像, 以及HPT前后的低密度的本征非晶硅的傅里叶红外光谱^[29]; (c) 对于各种a-Si:H钝化膜采用连续热退火工艺(Δn = 10¹⁵ cm^–3)的平均有效τ_eff和iV_oc^[33]; (d) 不同T和R_H下的单、双层i-a-Si:H结构的TEM图像^[33]; (e) 单层钝化的SHJ太阳电池结构图^[34]; (f)双层钝化的SHJ太阳电池结构图^[35]

Figure 3. (a) Changes of microstructural factor (R^*) and hydrogen content (C_H) of the film with hydrogen dilution ratio $ ({R_{\text{H}}} = {{{f_{{{\text{H}}_2}}}} {/} {{f_{{\text{Si}}{{\text{H}}_4}}}}}) $, where the gray area represents the amorphous-microcrystalline transition region^[27]; (b) HR-TEM images of the interface between i-a-Si and c-Si in the transition zone before and after HPT, as well as Fourier transform infrared spectra of low-density intrinsic amorphous silicon before and after HPT^[29]; (c) the average effective τ_eff and iV_oc of various a-Si:H passivation films using continuous thermal annealing process (Δn =10¹⁵ cm^–3)^[33]; (d) TEM images of single-layer and double-layer i-a-Si:H structures at various T and R_H levels^[33]; (e) structure diagram of SHJ solar cell with single-layer passivation^[34]; (f) structure diagram of SHJ solar cell with double-layer passivation^[35].

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图 4 (a) 不同沉积速率的i-a-Si:H相变为c-Si的临界温度^[40]; (b)两种沉积速率下不同衬底温度的有效τ_eff^[40]; (c) 不同i层厚度条件下的I-V性能^[41]; (d)不同i层厚度的SHJ太阳电池的内量子效率(IQE)图, 其中参考电池为p型扩散结电池^[41]; (e) 不同氢气流量(f_H)下的τ_eff和C_H, 插图显示了钝化结构^[42]; (f) 不同R_H下i-a-Si:H钝化c-Si的有效τ_eff, 且τ_eff随退火温度变化^[27]; (g) 上图为不同FR下i-a-Si:H层钝化c-Si的τ_eff, 下图为30 cm/min (标准状况)的FR放电的光学发射光谱(OES). 插图为在不同气体FR下的SiH^*的积分强度^[43]; (h) 不同衬底温度T下的τ_eff和iV_oc^[44]; (i) c-Si/a-Si:H界面能带图和载流子动力学示意图, 左图和右图分别对应宽带隙(E_g)的a-Si:H和窄带隙的a-Si:H^[44]

Figure 4. (a) Critical temperatures for the phase transition from i-a-Si:H to c-Si at different deposition rates^[40]; (b) effective τ_eff at various substrate temperatures for two deposition rates^[40]; (c) I-V performance under different i-layer thicknesses^[41]; (d) internal quantum efficiency (IQE) maps of SHJ solar cells with various i-layer thicknesses, with a reference cell being a p-type diffused junction cell^[41]; (e) τ_eff and C_H under different hydrogen flow rates (f_H), inset showing the passivation structure^[42]; (f) effective τ_eff for i-a-Si:H passivating c-Si under different R_H, with τ_eff varying with annealing temperature^[27]; (g) τ_eff of c-Si passivated by i-a-Si:H layers at different FR (up), optical emission spectrum (OES) spectrum of FR discharge at 30 cm/min under standard temperature and pressure (down), the inset shows the integrated intensity of SiH^* under different FR^[43]; (h) τ_eff and iV_oc at various substrate temperatures T^[44]; (i) energy band diagram and carrier dynamics schematic at the c-Si/a-Si:H interface, with the left and right figures corresponding to wide bandgap (E_g) a-Si:H and narrow bandgap a-Si:H, respectively^[44].

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图 5 (a) 在退火过程中a-Si:H基体内部微观变化的3个阶段(I, II, III)示意图, 每个阶段分为3个部分, 分别为c-Si/a-Si:H界面、a-Si:H膜的基体内部和a-Si:H表面处, 且c-Si/a-Si:H界面处的椭圆体表示未钝化的悬挂键^[45]; (b) 不同注入水平下, 有I-HPT和无HPT的有效寿命τ_eff的比较^[37]; (c) 左图为微波处理的前后τ_eff的变化, 右图为归一化τ_eff与微波处理周期数的关系^[34]

Figure 5. (a) Schematic illustration of three stages (I, II, III) of microstructural changes within the a-Si:H matrix during annealing, each stage divided into three parts: c-Si/a-Si:H interface, interior of the a-Si:H film, and a-Si:H surface, ellipsoids at the c-Si/a-Si:H interface represent unpassivated dangling bonds^[45]; (b) comparison of effective lifetimes (τ_eff) between I-HPT and No-HPT at different injection levels^[37]; (c) left: changes in τ_eff before and after microwave treatment; right: relationship between normalized τ_eff and the number of microwave treatment cycles^[34].

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图 6 (a) 用i-a-Si:H/n-a-Si:H钝化的c-Si(n)的τ_eff值与n-a-Si:H厚度的关系^[46]; (b) n型SHJ太阳电池能带图^[23]; (c) 左图对应于10 nm厚度的致密i-a-Si:H, 分别被0, 6和10 nm厚度的n-a-Si:H沉积后的傅里叶红外光谱(FTIR), 右图为对应于10 nm厚度的低密度i-a-Si:H, 分别被0, 6和10 nm厚度的n-a-Si:H沉积后的FTIR^[46]; (d) 上图为在不同厚度下n-a-Si:H沉积过程中, 两种密度的i-a-Si:H的介电函数虚部的强度, 下图为拉曼强度的变化^[46]; (e) 分步退火温度对钝化质量的影响, 由在Fz-Si(n)表面上所沉积的本征和掺杂a-Si:H薄膜的有效表面复合速率(S_eff)和τ_eff表示^[50]; (f)线性梯度退火对a-Si:H薄膜中H₂逸出率的影响, 上方图为c-Si表面的H₂逸出率数据; 中间图为单层a-Si:H薄膜的H₂逸出率数据, 下方图为堆叠膜的H₂逸出率数据^[50]; (g) 测试结构的深度与硼浓度的关系, 插图为测试所用结构, 且退火条件与图(e)的条件相同^[50]

Figure 6. (a) Relationship between the τ_eff value of c-Si(n) passivated with i-a-Si:H/n-a-Si:H and the thickness of n-a-Si:H^[46]; (b) energy band diagram of an n-type SHJ solar cell^[23]; (c) Fourier transform infrared spectroscopy (FTIR) spectra of 10 nm thick dense i-a-Si:H deposited with 0, 6, and 10 nm thick n-a-Si:H, respectively (left), FTIR spectra of 10 nm thick low-density i-a-Si:H deposited with 0, 6, and 10 nm thick n-a-Si:H, respectively (right); (d) intensity of the imaginary part of the dielectric function of two densities of i-a-Si:H during n-a-Si:H deposition at various thicknesses (up), changes in Raman intensity (down)^[46]; (e) impact of stepwise annealing temperatures on passivation quality, represented by the effective surface recombination velocity (S_eff) and τ_eff of intrinsic and doped a-Si:H films deposited on Fz-Si(n) surfaces; (f) influence of linear gradient annealing on the H₂ evolution rate in a-Si:H films, with upper panel showing H₂ evolution rate data on c-Si surfaces, middle panel for single-layer a-Si:H films, and lower panel for stacked films; (g) depth profile of boron concentration in the tested structure shown, with the inset illustrating the tested structure used and the annealing conditions identical to those in Fig. (e)^[50].

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图 7 (a) i-a-SiO_x:H材料原子结构示意图; (b) i-a-SiO_x:H钝化c-Si的微观结构示意图; (c) i-a-SiO_x:H钝化的SHJ太阳电池的器件结构图^[63]; (d)不同CO₂/SiH₄下的SHJ太阳电池的I-V性能^[63]; (e)左图为不同E_g下的i-a-Si:H层的SHJ太阳电池的能带图(如虚线所示, ΔE_V被放大并作为插图), 右图为不同E_g对SHJ电池的J_sc, V_oc和FF的影响^[66]; (f)优化后的3层a- SiO_x:H (i0, i1, i2) 的SHJ太阳电池的I-V性能与未优化a-Si:H (i0, i1, i2) 的SHJ太阳电池的I-V性能的比较^[67]; (g) 连续20 min退火后c-Si的有效τ_eff, 所述的钝化结构左侧图为两侧分别沉积不同$ {R_{{\text{C}}{{\text{H}}_{4}}}} $($ {R_{{\text{C}}{{\text{H}}_{4}}}} = {{{f_{{\text{C}}{{\text{H}}_{4}}}}} {/} {\left( {{f_{{\text{C}}{{\text{H}}_{4}}}} + {f_{{\text{Si}}{{\text{H}}_{4}}}}} \right)}} $) 的a-SiC_x:H膜, a-SiC_x:H膜的厚度为50 nm, 右侧图为背面沉积50 nm厚的a-Si:H膜, 正面沉积两层10 nm厚的本征a-SiC_x:H堆叠层, 其中R_CH4为0%或75%, 下方图为在适中温度下退火的第1阶段时, 这种堆叠层中氢运动的示意图(从左到右分别为0%/0%, 0%/75%, 75%/0%和75%/75%)^[62]

Figure 7. (a) Schematic illustration of the atomic structure of i-a-SiO_x:H material^[63]; (b) schematic diagram of the microstructure of c-Si passivated by i-a-SiO_x:H^[63]; (c) device structure diagram of the i-a-SiO_x:H passivated SHJ solar cell^[63]; (d) I-V performance of SHJ solar cells under different CO₂/SiH₄ ratios^[63]; (e) the left figure illustrates the band diagram of the SHJ solar cell with an a-Si:H(i) layer featuring various E_g, where the deviation of the valence band (ΔE_V) is zoomed in and presented as an inset (indicated by dashed lines), the right figure demonstrates the simulated impact of different E_g values on the J_sc, V_oc, and FF of the SHJ solar cell^[66]; (f) comparison of the I-V performance between optimized triple-layer a-SiO_x:H (i0, i1, i2) and unoptimized a-Si:H (i0, i1, i2) passivated SHJ solar cells^[67]; (g) effective τ_eff of c-Si after continuous annealing for 20 min. the passivation structures are described as follows, the left figure shows a-SiC_x:H films with different $ {R_{{\text{C}}{{\text{H}}_{4}}}} $ ($ {R_{{\text{C}}{{\text{H}}_{4}}}} = {{{f_{{\text{C}}{{\text{H}}_{4}}}}} {/} {\left( {{f_{{\text{C}}{{\text{H}}_{4}}}} + {f_{{\text{Si}}{{\text{H}}_{4}}}}} \right)}} $) deposited on both sides, with a thickness of 50 nm for the a-SiC_x:H films. the right figure depicts a 50 nm thick a-Si:H film deposited on the back and a two-layer stack of 10 nm thick intrinsic a-SiC_x:H films on the front, with ${R_{{\text{C}}{{\text{H}}_{4}}}} $ set at 0% or 75%, the bottom figure illustrates the schematic of hydrogen movement within this stacked layer during the first stage of annealing at a moderate temperature (from left to right was 0%/0%, 0%/75%, 75%/0%, and 75%/75%)^[62].

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图 8 (a)实验批次中性能最佳的SHJ电池的I-V曲线, 以及随着DH85持续时间变化, 各组电池PCE, J_sc, V_oc, FF和R_s的相对变化^[68]; (b)钠离子老化试验中裸露的SHJ太阳电池参数退化百分比和钠离子老化试验前后裸露的SHJ太阳电池的光致发光(PL)图像^[36]; (c) 在钠离子老化试验中, 带有80 nm厚SiO_x层的SHJ太阳电池参数退化百分比和钠离子老化试验前后, 带有80 nm厚SiO_x层的SHJ太阳电池的PL图像^[36]; (d) SHJ太阳能电池在UV照射和LS处理循环过程中的归一化性能变化^[71]

Figure 8. (a) I-V curve of the champion SHJ cell from the experiment batch, and relative changes in PCE, J_sc, V_oc, FF, and R_s as a function of DH85 duration for each group^[68]; (b) percentage degradation of parameters for exposed SHJ solar cells during sodium ion aging tests, along with Photoluminescence (PL) images of the exposed SHJ solar cells before and after the sodium ion aging tests^[36]; (c) percentage degradation of parameters for SHJ solar cells with an 80-nm-thick SiO_x layer during sodium ion aging tests, along with PL images of the SHJ solar cells with an 80-nm-thick SiO_x layer before and after the sodium ion aging tests^[36]; (d) normalized performance changes of SHJ solar cells during UV irradiation and LS treatment cycles^[71].

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图 9 (a) TOPCon太阳能电池结构图^[73]; (b) 载流子通过TOPCon太阳电池隧穿氧化物传输的能带图^[73]; (c) TOPCon界面钝化的iV_oc作为退火温度的函数, 没有隧穿氧化物(红色圆圈)的样品清楚地强调了隧穿氧化物层对于表面钝化的重要性^[72]; (d) 不同通源时间下制备的 TOPCon 太阳电池的E_ff和V_oc^[78]; (e) 不同厚度i-a-Si:H退火过程中磷向Si衬底中的扩散示意图, i-a-Si:H的厚度分别为0, 10, 20, 30和40 nm, 对应于对照组、G1组、G2组、G3组和G4组^[10]; (f) 采用p-a-Si:H的TOPCon太阳电池示意图^[84]; (g) 采用和未采用p-a-Si:H的TOPCon太阳电池的有效τ_eff曲线与Δn的函数关系^[84]; (h) J-V特性曲线^[84]; (i) EQE曲线^[84]

Figure 9. (a) Schematic diagram of the TOPCon solar cell structure^[73]; (b) energy band diagram illustrating carrier transport through the tunnel oxide in a TOPCon solar cell^[73]; (c) the iV_oc of TOPCon interface passivation as a function of annealing temperature, the sample without a tunneling oxide layer (red circles) clearly emphasizes the importance of the tunneling oxide layer for surface passivation^[72]; (d) the E_ff and V_oc of TOPCon solar cells prepared under different exposure times to the dopant source^[78]; (e) illustration of phosphorus diffusion into the Si substrate during the annealing process for various thicknesses of i-a-Si:H. the thicknesses of i-a-Si:H are 0, 10, 20, 30, and 40 nm, corresponding to the control group, Group G1, Group G2, Group G3, and Group G4, respectively^[10]; (f) schematic of a TOPCon solar cell employing p-a-Si:H^[84]; (g) effective τ_eff curves as a function of Δn for TOPCon solar cells with and without p-a-Si:H^[84]; (h) J-V characteristic curves^[84]; (i) EQE curves^[84].

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图 10 (a) p型PERC太阳能电池的结构图^[93]; (b) 与Al₂O₃和p-Si衬底相关的钝化机制^[93]; (c) 5层和单层SiN_x:H薄膜太阳电池的效率比较, 单层SiN_x:H膜的厚度为150 nm, 而5层膜的厚度为20/10/10/10/100 nm^[94]

Figure 10. (a) Schematic diagrams of structure of p-type PERC solar cell^[93]; (b) mechanism of passivation correlated with Al₂O₃ and p-Si substrate^[93]; (c) efficiency comparison for the solar cells with five-layer and single layer SiN_x:H films. the thickness of the single-layer SiN_x:H film is 150 nm, and the thicknesses for the five-layer films are 20/10/10/10/100 nm^[94].

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表 1 不同R_H的i-a-Si:H薄膜的特征参数^[33]

Table 1. Characteristic parameters of i-a-Si:H thin films with different R_H^[33].

R_H	SiH₄ flow/ sccm	H₂ flow/ sccm	R^*	τ_eff/μs	iV_oc/mV
纯 c-Si	—	—	—	0.98	520
R_H = 1	40	40	0.970	8.2	538
R_H = 10	40	400	0.143	148.1	668
R_H = 25	40	1000	0.076	127.1	661

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表 2 具有不同R_H的界面层和覆盖层的i-a-Si:H双层钝化性能参数^[33]

Table 2. Performance parameters of i-a-Si:H double- layer passivation with interface and cover layers with different R_H^[33].

双层钝化(c-Si/界面层/覆盖层)	τ_eff/μs	iV_oc/mV
c-Si/i-a-Si:H(R_H = 1)/ i-a-Si:H(R_H = 10)	33.9	606
c-Si/i-a-Si:H(R_H = 25)/ i-a-Si:H(R_H = 10)	138.9	665
c-Si/i-a-Si:H(R_H = 10)/ i-a-Si:H(R_H = 25)	197.6	683

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表 3 具有单层和双层钝化结构的SHJ器件性能

Table 3. Performance of SHJ devices with single- and double-layer passivation structures.

结构	J_sc/(mA·cm^–2)	V_oc/mV	FF/%	η/%	Year	Ref.
单层	39.02	735.1	77.57	22.23	2022	[36]
单层	36.50	718.0	77.50	20.30	2023	[37]
单层	39.60	735.0	79.00	23.00	2024	[34]
双层	38.90	741.0	80.60	23.20	2019	[38]
双层	39.50	747.0	84.98	25.11	2020	[39]
双层	40.27	749.7	85.90	25.92	2024	[35]

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表 4 不同SiO_x生长方法的器件应用

Table 4. Application of devices with different SiO_x growth methods.

生长方法	J_sc/(mA·cm^–2)	V_oc/mV	FF/%	η/%	Year	Ref.
热氧化	40.0	689.4	81.35	22.43	2020	[74]
PECVD	41.43	713.2	84.55	25.06	2023	[75]
化学氧化	41.38	730.8	81.9	24.8	2023	[76]
臭氧氧化	41.03	702.0	83.35	24.08	2024	[77]

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表 5 高性能TOPCon太阳电池结构比较^[79]

Table 5. Comparison of high performance TOPCon solar cells structures.

c-Si	Cell structure	V_oc/mV	J_sc/(mA·cm^–2)	FF/%	η/%	Ref.
n	Metal/SiN_x+MgF₂/Al₂O₃/p⁺-Siemitter/n-c-Si/SiO_x/n⁺-poly Si layer/Metal(n-TOPCon)	724.9	42.5	83.3	25.7	[80]
p	Metal/SiN_x/P-doped emitter/p-c-Si/SiO_x/B-doped p-poly Si layer/Metal(p-TOPCon)	701	41.1	79.9	23	[81]
p	Metal/SiN_x-MgF₂/Al₂O₃/p⁺-Si/p-c-Si/SiO_x/	714.2	42.4	80.8	24.3	[82]
p	P-doped n-poly Si layer/Metal(TOPCoRE)Metal/SiN_x/Al₂O₃/ B-diffusion FSF/p-c-Si/SiO_x/P-doped n-poly Si layer/ Metal (TOPCoRE)	732.3	42.05	84.3	26	[83]

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表 6 改进TOPCon太阳电池性能的方法

Table 6. Methods for improving TOPCon solar cells performance.

改善方法	J_sc/(mA·cm^–2)	V_oc/mV	FF/%	η/%	Year	Refs.
生长两步氧化	41.80	707.0	83.0	24.60	2022	[85]
正面金属电极和硼发射极之间沉积局部p-a-Si:H	42.03	696.0	83.76	24.50	2024	[84]
在钝化层中插入本征非晶硅(i-a-Si:H)层	40.60	715.0	82.30	23.83	2024	[10]
利用管式PECVD制备掺C poly-Si(n+)	40.81	700.4	82.70	23.64	2024	[86]
RS-ALD法制备高质量Al₂O₃薄膜	—	736.3	84.05	25.78	2024	[87]
中温光浸泡工艺	42.10	729.0	84.0	25.80	2024	[88]

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表 7 改进PERC太阳电池钝化性能的方法

Table 7. Methods for improving passivation performance of PERC solar cells.

改善方法	J_sc/(mA·cm^–2)	V_oc/mV	FF/%	η/%	Year	Ref.
利用臭氧氧化制备氧化铝层	37.89	590	75.70	16.92	2020	[95]
5层 SiN_x:H 薄膜	10.273	681.63	81.19	22.56	2021	[94]
背面以 H_fO₂ 作为钝化材料钝化	39.67	662.9	79.26	20.84	2022	[93]
离子注入SiO_x N_y:H	40.80	686	81.54	22.80	2022	[96]
发射极表面通过硫化氢(H₂S)气体反应钝化	40.03	649	76.79	19.93	2023	[97]
利用SiO₂/Al₂O₃双层钝化	38.73	649	79.00	19.90	2024	[98]
多层SiN_x/SiO_xN_y/SiN_x钝化	41.70	682	80.57	22.91	2024	[99]

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