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Impact of oxygen incorporation on interface optimization and defect suppression for efficiency enhancement in Cu2ZnSn（S,Se）4 solar cells

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Journal of Energy Chemistry 2024年第8期95卷 77-85页

作者： Shicheng Deng Songfan Wang Yuanyuan Wang Qian Xiao Yuena Meng Dongxing Kou Wenhui Zhou Zhengji Zhou Zhi Zheng sixin wu Key Laboratory for Special Functional Materials of MOE National & Local Joint Engineering Research Centre for High-efficiency Display and Lighting TechnologySchool of Materials Henan University Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province Institute of Surface Micro and Nano Materials College of Chemical and Materials Engineering Xuchang University

Kesterite Cu2ZnSn（S,Se）4（CZTSSe） solar cells suffer from severe carrier recombination, limiting the photovoltaic performance. Unfavorable energy band alignment at the p-n junction and defective front interface are two main causes. Herein, oxygen incorporation in CZTSSe via absorber air-annealing was developed as a strategy to optimize its surface photoelectric property and reduce the defects. With optimized oxygen incorporation conditions, the carrier separation and collection behavior at the front interface of the device is improved. In particular, it is found that oxygen incorporated absorber exhibits increased band bending, larger depletion region width, and suppressed absorber defects. These indicate the dynamic factors for carrier separation become stronger. Meanwhile, the increased potential difference between grain boundaries and intra grains combined with the decreased concentration of interface deep level defect in the absorber provide a better path for carrier transport. As a consequence, the champion efficiency of CZTSSe solar cells has been improved from 9.74% to 12.04% with significantly improved open-circuit voltage after optimized air-annealing condition. This work provides a new insight for interface engineering to improve the photoelectric conversion efficiency of CZTSSe devices.

关键词： Defect suppression Interface optimization Kesterite Surface oxidation Thin film solar cell

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Surface defect ordered Cu_(2)ZnSn(S,Se)_(4) solar cells with efficiency over 12% via manipulating local substitution

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Journal of Energy Chemistry 2022年第4期31卷 555-562页

作者： Changcheng Cui Dongxing Kou Wenhui Zhou Zhengji Zhou Shengjie Yuan Yafang Qi Zhi Zheng sixin wu Key lab for Special Functional Materials Ministry of EducationNational&Local Joint Engineering Research Center for High-Efficiency Display and Lighting TechnologySchool of Materials Science and EngineeringCollaborative Innovation Center of Nano Functional Materials and ApplicationsHenan UniversityKaifeng 475004HenanChina Inst Surface Micro&Nano Mat Coll Adv Mat&EnergyKey Lab Micronano Energy Storage&Convers Mat HeXuchang UniversityXuchang 461000HenanChina

The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large open-circuit voltage deficit(V_(oc,deficit)) and significantly limit kesterite photovoltaics performance,primarily arising from the generated more recombination centers and insufficient p to n conversion at p-n junction. Herein, we establish a surface defects ordering structure in CZTSSe system via local substitution of Cu by Ag to suppress disordered Cu_(Zn) defects and generate benign n-type Zn_(Ag) donors. Taking advantage of the decreased annealing temperature of Ag F post deposition treatment(PDT), the high concentration of Ag incorporated into surface absorber facilitates the formation of surface ordered defect environment similar to that of efficient CIGS PV. The manipulation of highly doped surface structure could effectively reduce recombination centers, increase depletion region width and enlarge the band bending near p-n junction. As a result, the Ag F-PDT device finally achieves maximum efficiency of 12.34% with enhanced V_(oc) of 0.496 V. These results offer a new solution route in surface defects and energy-level engineering, and open the way to build up high quality p-n junction for future development of kesterite technology.

关键词： Kesterite Cu_(2)ZnSn(S,Se)_(4)thin film solar cells Interface recombination Defect passivation Ag substitution

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Highly efficient solution-processed CZTSSe solar cells based on a convenient sodium-incorporated post-treatment method

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Journal of Energy Chemistry 2020年第1期29卷 196-203,I0007页

作者： Biwen Duan Linbao Guo Qing Yu Jiangjian Shi Huijue wu Yanhong Luo Dongmei Li sixin wu Zhi Zheng Qingbo Meng Key Laboratory for Renewable Energy(CAS) Beijing Key Laboratory for New Energy Materials and DevicesInstitute of PhysicsChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Songshan Lake Materials Laboratory Dongguan 523808GuangdongChina Key Laboratory for Special Functional Materials of MOE Henan UniversityKaifeng 475004HenanChina Key Laboratory for Miao-Nano Energy Storage and Conversion Materials of Henan Province College of Advanced Materials and EnergyInstitute of Surface Micro and NanomaterialsXuchang UniversityXuchang 461000HenanChina

In CZTSSe solar cells,a simple sodium-incorporation post-treatment method toward solution-processed Cu2Zn Sn S4precursor films is presented in this work.An ultrathin NaCl film is deposited on Cu2Zn Sn S4precursor films by spin-coating NaCl solution.In subsequent selenization process,the introduction of Na Cl is found to be benefacial for the formation of Cu2-xSe,which can further facilitate the element transportation,leading to dense and smooth CZTSSe films with large grains and less impurity Cu2Sn(S,Se)3phase.SIMS depth profiles confirm the gradient distribution of the sodium element in Na-doped absorbers.Photoluminescence spectra show that the introduction of appropriate sodium into the absorber can inhibit the band tail states.As high as 11.18% of power conversion efficiency(PCE)is achieved for the device treated with 5 mg mL^-1 NaCl solution,and an average efficiency of Na-doped devices is 10.71%,13%higher than that of the control groups(9.45%).Besides,the depletion width and the charge recombination lifetime can also have regular variation with sodium treatment.This work offers an easy modification method for high-quality Na-doped CZTSSe films and high-performance devices,in the meantime,it can also help to further understand the effects of sodium in CZTSSe solar cells.

关键词： Thin film solar cell CZTSSe Sodium doping Post-treatment Spin-coating method

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Lithium-assisted synergistic engineering of charge transport both in GBs and GI for Ag-substituted Cu2ZnSn(S,Se)4 solar cells

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Journal of Energy Chemistry 2020年第11期29卷 9-15页

作者： Xiangyun Zhao Xiaohuan Chang Dongxing Kou Wenhui Zhou Zhengji Zhou Qingwen Tian Shengjie Yuan Yafang Qi sixin wu The authors contributed equally to this work Key Lab for Special Functional MaterialsMinistry of EducationNational&Local Joint Engineering Research Center for High-Efficiency Display and Lighting TechnologySchool of Materials Science and EngineeringCollaborative Innovation Center of Nano Functional Materials and ApplicationsHenan UniversityKaifeng 475004HenanChina

Although silver(Ag) substitution offers several benefits in eliminating bulk defects and facilitating interface type inversion for Cu2ZnSn(S,Se)4(CZTSSe) photovoltaic(PV) technology, its further development is still hindered by the fairly low electrical conductivity due to the significant decrease of acceptors amount.In this work, a versatile Li–Ag co-doping strategy is demonstrated to mitigate the poor electrical conductivity arising from Ag through direct incorporating Li via postdeposition treatment(PDT) on top of the Ag-substituted CZTSSe absorber. Depth characterizations demonstrate that Li incorporation increases ptype carrier concentration, improves the carrier collection within the bulk, reduces the defects energy level as well as inverts the electric field polarity at grain boundaries(GBs) for Ag-substituted CZTSSe system. Benefiting from this lithium-assisted complex engineering of electrical performance both in grain interior(GI) and GBs, the power conversion efficiency(PCE) is finally increased from 9.21% to 10.29%. This systematic study represents an effective way to overcome the challenges encountered in Ag substitution,and these findings support a new aspect that the synergistic effects of double cation dopant will further pave the way for the development of high efficiency kesterite PV technology.

关键词： Cu2ZnSn(S,Se)4 Thin film solar cell Ag substitution Alkali doping Post-treatment

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Adjusting the SnZn defects in Cu_(2)ZnSn(S,Se)_(4) absorber layer via Ge^(4+) implanting for efficient kesterite solar cells

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Journal of Energy Chemistry 2021年第10期30卷 1-7,I0001页

作者： Yueqing Deng Zhengji Zhou Xin Zhang Lei Cao Wenhui Zhou Dongxing Kou Yafang Qi Shengjie Yuan Zhi Zheng sixin wu Key Lab for Special Functional Materials Ministry of EducationNational and Local Joint Engineering Research Center for High-Efficiency Display and Lighting TechnologyAnd School of MaterialsHenan UniversityKaifeng 475004HenanChina Collaborative Innovation Centre of Nano Functional Materials and Applications HenanChina Key Laboratory for Micro-Nano Energy Storage and Conversion Materials of Henan Province College of Advanced Materials and EnergyInstitute of Surface Micro and Nano MaterialsXuchang UniversityXuchang 461000HenanChina

The development of kesterite photovoltaic solar cells has been hindered by large open-circuit voltage(V_(oc))deficit.Recently,Snzn deep point defect and associative defect cluster have been recognized as the main culprit for the Voc losses.Therefore,manipulating the deep-level donor of Snzn antisite defects is crucial for breaking through the bottleneck of present Cu_(2) ZnSn(S,Se)_(4)(CZTSSe)photovoltaic technology.In this study,the Snzn deep traps in CZTSSe absorber layer are suppressed by incorporation of Ge.The energy levels and concentration of Snzn defects measured by deep-level transient spectroscopy(DLTS)decrease significantly.In addition,the grain growth of CZTSSe films is also promoted due to Ge implantation,yielding the high quality absorber layer.Consequently,the efficiency of CZTSSe solar cells increases from 9.15%to 11.48%,largely attributed to the 41 mV Voc increment.

关键词： CZTSSe Defect Absorber layer Solar cells V_(oc)

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Enhancing Grain Growth for Efficient Solution-Processed (Cu,Ag)2ZnSn(S,Se)4 Solar Cells Based on Acetate Precursor

Enhancing Grain Growth for Efficient Solution-Processed (Cu,...

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第七届新型太阳能电池材料科学与技术学术研讨会

作者： Yafang Qi sixin wu Henan University

Material crystallinity is the overriding factor in the determination of the photoelectric properties of absorber materials and the overall performance of photovoltaic device.Nevertheless,in Cu2 Zn Sn(S,Se)4(CZTSSe) photovoltaic device the bilayer or tri-layer structure for the absorber have been broadly observed,which are generally harmful to the cell performance due to the probability of photogenerated carrier recombination at grain boundaries significantly increased.1-4 Herein,our experiment reveals that application of anions to a new family of(Cu,Ag)2 Zn Sn(S,Se)4(CAZTSSe) materials leads to the increase of grain size and crystallinity.It is inspiring that by using acetate starting materials in precursor solution,a uniform,compact and pinhole-free CAZTS precursor film was obtained,and the smoothness of the films surpassed that of films fabricated from oxide route.More importantly,the crystallization of the CAZTSSe film has been considerably enhanced after selenization,large grains go through the entire absorber layer was successfully obtained.Additionally,it is observed that the Voc accompanied by excellent crystallinity improved significantly due to the pronouncedly reduced carrier recombination loss at grain boundaries.As a consequence,the power conversion efficiency(PCE) of the CAZTSSe photovoltaic device is successfully increased from 10.35%(oxide route) to 11.32%(acetate route).Importantly,our work attest to the feasibility of tuning the crystallization of the CZTSSe film by simple chemistry.

关键词： CAZTSSe solar cell anion acetate starting material crystallization recombination

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Metal–organic framework wafer enabled fast response radiation detection with ultra-low dark current

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Nano Research 2024年第4期17卷 2988-2993页

作者： Meng Xu Jianxi Liu Wei wu Yang Chen Donghao Ma sixin Chen Wanqi Jie Menghua Zhu Yadong Xu State Key Laboratory of Solidification Processing MIIT Key Laboratory of Radiation Detection Materials and Devices&School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

Semiconductive metal–organic frameworks(MOFs)have attracted great interest for the electronic applications.However,dark currents of present hybrid organic–inorganic materials are 1000–10,000 times higher than those of commercial inorganic detectors,leading to poor charge transportation.Here,we demonstrate a ZIF-8(Zn(mim)_(2),mim=2-methylimidazolate)wafer with ultra-low dark current of 1.27 pA·mm^(-2) under high electric fields of 322 V·mm^(-1).The isostatic pressing preparation process provides ZIF-8 wafers with good transmittance.Besides,the presence of redox-active metals and small spatial separation between components promotes the charge hopping.The ZIF-8-based semiconductor detector shows promising X-ray detection sensitivity of 70.82μC·Gy^(-1)·cm^(-2) with low doses exposures,contributing to superior X-ray imaging capability with a relatively high spatial resolution of 1.2 lp·mm^(-1).Simultaneously,good peak discrimination with the energy resolution of~43.78%is disclosed when the detector is illuminated by uncollimated 241Am@5.48 MeVα-particles.These results provide a broad prospect of MOFs for future radiation detection applications.

关键词： MOFs lead-free α-particles X-ray detection and imaging dark current fast response

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Highly luminescent ZnO and CdS nanostructures prepared by ionic liquid precursors

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Science China Chemistry 2009年第12期52卷 2141-2147页

作者： TAO LeiMing XU HongTao AN YanQing DU ZuLiang wu sixin Key Laboratory for Special Functional Materials of Ministry of Education Henan UniversityKaifeng 475004China

The ionic liquids containing Cd and Zn,which served as the metal-chalcogenides precursors,were synthesized and reacted with Na2S to synthesize the ionic-liquid-capped semiconductors. The products were detected by XRD and TEM. The results demonstrated that the CdS was composed of 5―6 nm monodispersed nanocrystals. At the same time,the ZnO composed of 1 μm hexagonal-disk nanostructure was prepared under the same experimental condition. The difference of the morphology and structures between Zn and Cd systems was discussed by thermodynamics and crystallography. The fluorescence of as-prepared ZnO and CdS showed the excellent photoluminescence.

关键词： ionic-liquid ZnO CdS

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Solvent-free Synthesis of Hexagonal Iron Sulfide Nanoflowers

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Chinese Journal of Chemistry 2013年第8期31卷 983-986页

作者： Xia Wang Wenhui Zhou Zhixian Chang Zhengji Zhou sixin wu The Key Laboratory for Special Functional Materials of MOE Henan University Kaifeng Henan 475004 China

采用绿色和经济没有溶剂的合成线路，六角形的铁硫化物(Fe7S8 ) nanoflowers 成功地第一次被综合。在实验，铁的 hexadecylxanthate 被用作先锋，并且六角形的铁硫化物(Fe7S8 ) nanoflowers 被先锋的热分解在 260 点获得吗？

关键词：无溶剂合成纳米材料硫化铁透射电子显微镜扫描电子显微镜惰性气体保护合成路线六方晶系

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Efficiency enhancement of CZTSSe solar cells by cation substitution

Efficiency enhancement of CZTSSe solar cells by cation subst...

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第四届新型太阳能电池学术研讨会

作者： sixin wu Yafang Qi Jie Fu Jing Guo Yingli Pei Henan University

The development of kesterite CuZnSn(S,Se) thin-film solar cells is hindered by the large deficit of open-circuit voltage,which results from the easy formation of CuZn antisite acceptor defects.Suppressing the formatio...

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