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Double Layer Composite Electrode Strategy for Efficient Perovskite Solar Cells with Excellent Reverse-Bias Stability

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Nano-Micro Letters 2023年第1期15卷 225-235页

作者： Chaofan Jiang Junjie Zhou Hang Li Liguo Tan Minghao Li Wolfgang Tress Liming Ding Michael Grätzel Chenyi Yi State key laboratory of Power System Department of Electrical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China Institute of Computational Physics(ICP) ZHAW School of EngineeringWildbachstr.218400 WinterthurSwitzerland Center for Excellence in Nanoscience(cas) Key Laboratory of Nanosystem and Hierarchical Fabrication(CAS)National Center for Nanoscience and TechnologyBeijing 100190People’s Republic of China laboratory of Photonics and Interfaces Department of Chemistry and Chemical EngineeringSwiss Federal Institute of Technology Lausanne1015 LausanneSwitzerland

Perovskite solar cells(PSCs)have become the represent-atives of next generation of photovoltaics;nevertheless,their stability is insufficient for large scale deployment,particularly the reverse bias stability.Here,we propose a transparent conducting oxide(TCO)and low-cost metal composite electrode to improve the stability of PSCs without sacrificing the efficiency.The TCO can block ion migrations and chemical reactions between the metal and perovskite,while the metal greatly enhances the conductivity of the composite electrode.As a result,composite electrode-PSCs achieved a power conversion efficiency(PCE)of 23.7%(certified 23.2%)and exhibited excellent stability,maintaining 95%of the initial PCE when applying a reverse bias of 4.0 V for 60 s and over 92%of the initial PCE after 1000 h continuous light soaking.This composite electrode strategy can be extended to different combinations of TCOs and metals.It opens a new avenue for improving the stability of PSCs.

关键词： Composite electrode Perovskite solar cells Stability Reverse bias Characterization

Design and optical performance investigation of all-sprayable ultrablack coating

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Nano Research 2023年第12期16卷 12901-12909页

作者： Chen Shen Huiyong Li Shuai Sun Hui Zhang Lanqin Yan Zhong Zhang cas key laboratory of nanosystem and hierarchical fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education laboratory of Flexible Electronics Technology Department of ChemistryTsinghua UniversityBeijing 100084China cas key laboratory of Mechanical Behavior and Design of Materials Department of Modern MechanicsUniversity of Science and Technology of ChinaHefei 230027China

Although ultrablack surfaces are urgently needed in wide applications owing to their extremely low reflectance over a broadband wavelength,obtaining simultaneously the ultrablackness and mechanical robustness by simple process technique is still a great challenge.Herein,by decoupling different light extinction effects to different layers of coating,we design an ultrablack coating that is all-sprayable in whole process.This coating presents low reflectance over visible–mid-infrared(VIS–MIR)wavelength(av.R≈1%in VIS),low multi-angle scattering(bidirectional reflection distribution function(BRDF)=10-2–10-3 sr-1),together with good substrate adhesion grade and self-cleaning ability,which are superior to most reported sprayable ultrablack surfaces.The light extinction effects of each layer are discussed.This method is also applicable in other material systems.

关键词： ultrablack spray-coating carbon nanomaterials multiple scattering intermediate layer

100 cm^(2) Organic Photovoltaic Cells with 23%Efficiency under Indoor Illumination

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Chinese Journal of Polymer Science 2022年第8期40卷 979-988,I0011页

作者： Yong Cui Hui-Feng Yao Ye Xu Peng-Qing Bi Jian-Qi Zhang Tao Zhang Ling Hong Zhi-Hao Chen Zhi-Xiang Wei Xiao-Tao Hao Jian-Hui Hou laboratory of Polymer Physics and Chemistry Beijing National Laboratory for Molecular SciencesCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China cas key laboratory of nanosystem and hierarchical fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing100190China School of Physics State Key Laboratory of Crystal MaterialsShandong UniversityJinan250100China

The application of organic photovoltaic(OPV)cells to drive off-grid microelectronic devices under indoor light has attracted broad attention.As organic semiconductors intrinsically have less ordered intermolecular packing than inorganic materials,the relatively larger energetic disorder is one of the main results that limit the photovoltaic efficiency of the OPV cells at low carrier density.Here,we optimize the alkyl chains of non-fullerene acceptors to get suppressed energetic disorder.We find the optimal acceptor DTz-R1 with the shortest alkyl chain has the strongest crystalline property and lowest energetic disorder.As a result,over 26%efficiency is recorded for the 1 cm^(2) OPV cells under a light-emitting diode illumination of 500 lux.We also fabricate a 100 cm^(2) cell device and get a PCE of 23.0%,which is an outstanding value for large-area OPV cells.These results suggest that modulation of the energetic disorder is of great importance for further improving the efficiency of OPV cells,especially for indoor applications.

关键词： Organic photovoltaic cells Low light intensity Energetic disorder Energy loss Power conversion efficiency

Surface Passivation and Energetic Modification Suppress Nonradiative Recombination in Perovskite Solar Cells

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Nano-Micro Letters 2022年第7期14卷 32-42页

作者： Wei Dong Wencheng Qiao Shaobing Xiong Jianming Yang Xuelu Wang Liming Ding Yefeng Yao Qinye Bao Shanghai key laboratory of Magnetic Resonance East China Normal UniversityShanghai 200241People’s Republic of China School of Physics and Electronic Science East China Normal UniversityShanghai 200241People’s Republic of China Center for Excellence in Nanoscience(cas) Key Laboratory of Nanosystem and Hierarchical Fabrication(CAS)National Center for Nanoscience and TechnologyBeijing 100190People’s Republic of China Collaborative Innovation Center of Extreme Optics Shanxi UniversityTaiyuan 030006ShanxiPeople’s Republic of China

Surface passivation via post-treatment is an important strategy for improving power conversion efficiency and operational stability of perovskite solar cells.However,so far the interaction mechanisms between passivating additive and perovskite are not well understood.Here,we report the atomic-scale interaction of surface passivating additive 2,2-difluoroethylammonium bromine(2FEABr)on the MAPbI_(3).It is found that the bulky 2FEA+cations tend to distribute at film surface,while the Br−anions diffuse from surface into bulk.A combination of 19F,207Pb,and 2H solid-state NMR further reveal the Br−anions’partial substitution for the I−sites,the restricted motion of partial MA+cations,and the firmed perovskite lattices,which would improve charge transport and stability of the perovskite films.Optical spectroscopy and ultraviolet photoelectron spectroscopy demonstrate that the 2FEABr induced surface passivation and energetic modification suppress the nonradiative recombination loss.These findings enable the efficiency of the p-i-n structured PSC significantly increasing from 19.44 to 21.06%,accompanied by excellent stability.Our work further establishes more knowledge link between passivating additive and PSC performance.

关键词： Passivation Solid-state NMR Charge transport Perovskite solar cell

Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis

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Nano Research 2023年第12期16卷 12936-12941页

作者： Yang Gao Xiaohui Xu Yue Niu Xinran Hu Zeyu Li Longkun Yang Linjie Zhi Bin Wang cas key laboratory of nanosystem and hierarchical fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China The Beijing key laboratory for Nano-Photonics and Nano-Structure(NPNS) Department of PhysicsCapital Normal UniversityBeijing 100048China College of New Energy China University of Petroleum(East China)Qingdao 266580China

In comparison with the developing nano-carbon catalysts,some small organic molecules are also emerging as catalysts with typical features,however,their working mechanism is still unclear.Here,we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering.These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based H_(2)O_(2) electrosynthesis.Differing from the commonly reported carbon-based electrocatalysts,viologens can produce H_(2)O_(2) in a synergistic manner,which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator.We found that the ring current and H_(2)O_(2) selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group.As a result,a benzyl-substituted viologen(BV)delivers the best electrocatalytic performance among the samples,including the highest H_(2)O_(2) selectivity of 96.9%at 0.6 V and the largest ring current density of about 13.6 mA·mmol-1.Furthermore,density functional theory(DFT)calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital(HOMO)–lowest unoccupied molecular orbital(LUMO)energy gap of BV is beneficial to the synergistic mechanism for H_(2)O_(2) production.This work sheds new insight into the efficient H_(2)O_(2) production in a synergistic manner for small molecules-based electrocatalysts.

关键词： viologens electrocatalysis hydrogen peroxide redox mediator oxygen reduction

Single site catalyst with enzyme-mimic micro-environment for electroreduction of CO_(2)

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Nano Research 2022年第3期15卷 1817-1823页

作者： Chang Long Kaiwei Wan Xueying Qiu Xiaofei Zhang Jianyu Han Pengfei An Zhongjie Yang Xiang Li Jun Guo Xinghua Shi Hui Wang Zhiyong Tang Shaoqin Liu School of Materials Science and Engineering MOE Key Laboratory of Micro-systems and Micro-structures ManufacturingHarbin Institute of TechnologyHarbin150080China cas key laboratory of nanosystem and hierarchical fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing100190China University of Chinese Academy of Sciences Beijing100049China Institute of High Energy Physics cas Beijing100049China

Single site catalysts provide a unique platform for mimicking natural enzyme due to their tunable interaction between metal center and coordinated ligand.However,most works have focused on preparing structural and functional models of nature enzyme,with less reports also taking the local chemical environment,i.e.,functional/catalytic residues around the active site which is an essential feature of enzymes,into consideration.Herein,we report a Co-centered porphyrinic polymer containing the enzyme-mimic micro-environment,where the linker triazole over CoN4 site enables formation of hydrogen bond with the*COOH intermediate,thus promoting the electrocatalytic reduction of CO_(2).As-prepared catalyst achieves the CO_(2)-to-CO conversion of 5,788 h^(−1) turnover frequency value and near unit(~96%)faradaic efficiency at−0.61 V versus reversible hydrogen electrode.This strategy will bring new dimension of designing highly active single-site catalysts.

关键词： single-site catalyst CO_(2)electroreduction enzyme-mimic

Ethanol-derived white emissive carbon dots:The formation process investigation and multi-color/white LEDs preparation

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Nano Research 2022年第2期15卷 942-949页

作者： Boyang Wang Haoqiang Song Zhiyong Tang Bai Yang Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450001China cas key laboratory of nanosystem and hierarchical fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China State key Lab of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China

Carbon dots(CDs)have attracted much attention due to their excellent photoelectric properties and potential applications.Although previous studies have shown that almost all organic molecules can be converted into CDs via chemical carbonization,the mechanism of the conversion process remains unclear.The hydrothermal/solvothermal method commonly used to prepare CDs is complicated and leads to the generation of many by-product CDs with similar structures.Considering that the purification of the synthesized by-products is difficult,the process of CDs formation cannot be readily analyzed and understood.Herein,we use ethanol as a carbon source to synthesize white-emitting CDs(W-CDs).Column chromatography separation shows that the synthesized W-CDs are composed of blue-,cyan-,and yellow-emitting CDs that fluoresce at wavelengths corresponding to the three emission centers of W-CDs.Although the samples have similar graphitic structure,they exhibit different surface states due to variations in the degree of oxidation and carbonization.Therefore,the red-shift in their emission peaks is attributed to an increased degree of carbonization in their polymer structure.Theoretical calculations verify the experimental results,and the prepared CDs are successfully used to develop multi-color and white light-emitting diodes(LEDs).

关键词： carbon dots multi-color-emissive cross-linking fluorescence mechanism phosphors

11.39%efficiency Cu_(2)ZnSn(S,Se)_(4) solar cells from scrap brass

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SusMat 2022年第2期2卷 206-211页

作者： Yining Pan Chang Yan Xiangyun Zhao Wangxian Chen Kaiwen Sun Qing Wu Liming Ding Fangyang Liu School of Metallurgy and Environment Central South UniversityChangshaP.R.China Information and Network Centre Central South UniversityChangshaP.R.China Center for Excellence in Nanoscience(cas) Key Laboratory of Nanosystem and Hierarchical Fabrication(CAS)National Center for Nanoscience and TechnologyBeijingP.R.China

Kesterite Cu2ZnSn(S,Se)4(CZTSSe)is one of the most promising next-generation thin-film photovoltaic materials due to its environmental friendliness and earthabundant constitutions,excellent optoelectronic properties(high absorption coefficient>104/cm and tunable band gap 1.0–1.5 eV)and high theoretical efficiency(32%).1,2 In 2014,12.6%3 efficiency was achieved by the IBM group using the hydrazine method.Based on the sputtering process,12.62%4 efficiency for CZTSSe and 12.5%5 efficiency for CZTSe have been achieved in recent years.However,the highest efficiency has stuck around 12.6%for several years.Lately,a breakthrough with certified 13%power conversion efficiency(PCE)has been demonstrated for CZTSSe thin-film solar cells,surpassing the dust-covered efficiency record since 2014.3,6 Along with the efficiency advancement of kesterite solar cells,a cost-effective fabrication process with low carbon footprint plays an increasingly important role considering the near-future industrialisation of this kind of solar cell with low energy payback time.

关键词： CZTSSe kesterite scrap brass

Coordination-responsive drug release inside gold nanorod @ metal-organic framework core-shell nanostructures for near-infrared-induced synergistic chemo-photothermal therapy

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Nano Research 2018年第6期11卷 3294-3305页

作者： Yantao Li Jun Jin Dawei Wang Jiawei Lv Ke Hou Yaling Liu Chunying Chen Zhiyong Tang cas key laboratory of nanosystem and hierarchical fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Beijing 100190 China

Multifunctional core-shell nanostructures formed by integration of distinct components have received wide attention as promising biological platforms in recent years. In this work, crystalline zeolitic imidazolate framework-8 （ZIF-8）, a typical metal-organic framework （MOF）, is coated onto single gold nanorod （AuNR） core for successful realization of synergistic photothermal and chemotherapy triggered by near-infrared （NIR） light. Impressivel）~ high doxorubicin hydrochloride （DOX） loading capacity followed by pH and NIR light dual stimuli-responsive DOX release can be easily implemented through formation and breakage of coordination bonds in the system. Moreover, under NIR laser irradiation at 808 nm, these novel AuNR@MOF core-shell nanostructures exhibit effective synergistic chemo-photothermal therapy both in vitro and in vivo, confirmed by cell treatment and tumor ablation via intravenous injection.

关键词： core-shell nanostructures coordination bonds dual stimuli response synergistic cancer therapy