PbS quantum dot(QD)image sensors have emerged as promising chips for a wide range of infrared(IR)imaging applications due to their monolithic integration with silicon-based readout integrated circuits.However,avoiding...PbS quantum dot(QD)image sensors have emerged as promising chips for a wide range of infrared(IR)imaging applications due to their monolithic integration with silicon-based readout integrated circuits.However,avoiding primary toxic Pb usage and reducing the cost of PbS QDs remains crucial for widespread application.We present a novel cost-effective and environmentally friendly hydrometallurgical process for recovering PbCl_(2)from spent lead-acid battery paste to synthesize high-quality PbS QDs.The method recovers PbCl_(2)with a production ratio of 97%and a purity of 99.99%.PbS QDs and photodetectors synthesized from recycled PbCl_(2)(R-PbCl_(2))have comparable performance and quality to those made using commercial PbCl_(2).R-PbCl_(2)-derived photodetectors exhibit a high external quantum efficiency of 49.6%and a high specific detectivity of 6.95×10^(12)Jones compared to published studies.Additionally,based on R-PbCl_(2),a PbS QD image sensor with 640×512 resolution successfully discriminated common solvents.Moreover,through life-cycle assessment and economic cost analysis,this novel synthesis route offers great advantages in the environmentally friendly use of chemical reagents and reduces the production cost of PbS QDs by 23.2%compared to commercial PbCl_(2).Thus,this work not only contributes to the green recycling of spent lead paste but also provides a low-cost strategy for synthesizing PbS QDs and their optoelectronic application.展开更多
The bulky footprint of near-infrared(NIR)spectrometers has been limiting their applications in portable and movable systems for probing molecular compositions and structures.Quantum dot(QD)computational spectrometers ...The bulky footprint of near-infrared(NIR)spectrometers has been limiting their applications in portable and movable systems for probing molecular compositions and structures.Quantum dot(QD)computational spectrometers are a promising strategy for miniaturized NIR spectrometers,whose performance is limited by the poor spectral encoding matrix and,ultimately,the poor quality of PbS QDs.Here,we show that the monodispersity and finely controlled absorption peak of PbS QDs are critical parameters affecting the spectral resolution and noise resistance.Thus,a facile synthesis of a series of monodisperse PbS QDs from a single batch is developed using cation exchange synthesis in a seeded-growth manner.All the as-synthesized PbS QDs have narrow size distributions of below 4%,and the peak intervals can be controlled to within 3 nm.Furthermore,stable PbS QD inks are prepared by considering the compatibility between QD ligands,solvents,and polymers.The PbS QD filter array is fabricated using a contact printing method,exhibiting supreme transmittance curves and a spectral encoding matrix.The filter array is coupled with an InGaAs image sensor to form the QD NIR computational spectrometer.Thanks to the high-quality PbS QDs,the QD spectrometer shows a high spectral resolution of 1.5 nm in a broad wavelength range of 900−1700 nm and excellent spectral reconstruction of narrow and broad spectra with fidelities of above 0.987.Additionally,the QD spectrometer is applied to distinguish materials and accurately measure the alcohol content of white wines,demonstrating the great potential for practical applications of QD NIR spectrometers.展开更多
Stability under light is critical for lead sulfide quantum dots(PbS QDs)in solar cell applications.To improve the stability of PbS QDs solar cells,the influence of the light illumination on the performance of the as-p...Stability under light is critical for lead sulfide quantum dots(PbS QDs)in solar cell applications.To improve the stability of PbS QDs solar cells,the influence of the light illumination on the performance of the as-prepared PbS QDs solar cells was carefully investigated.Combined with X-ray and ultraviolet photoelectron spectroscopies,it was revealed that the 1,2-ethanedithiol(EDT)ligands of the hole transport p-type PbS QDs reacted with the ligands of the PbS QDs active layer under light illumination.The reaction not only undermines the n-type characteristics of the active layer,but also increases the number of defects,leading to a serious deterioration in device performance.An interface layer was introduced to block the EDT penetration to avoid this issue,significantly improving the stability of the device under light irradiation.Moreover,the separation of carriers was also enhanced due to the better matching the energy level of the interface layer.The device with an interface layer yielded a power conversion efficiency of 12.55%and sustained to a long time light illumination.展开更多
基金supported by Key program of National Natural Science Foundation of China(52330004)National Natural Science Foundation of China General Project(51978301)National Key Research and Development Program of China(2023YFC3902802)。
文摘PbS quantum dot(QD)image sensors have emerged as promising chips for a wide range of infrared(IR)imaging applications due to their monolithic integration with silicon-based readout integrated circuits.However,avoiding primary toxic Pb usage and reducing the cost of PbS QDs remains crucial for widespread application.We present a novel cost-effective and environmentally friendly hydrometallurgical process for recovering PbCl_(2)from spent lead-acid battery paste to synthesize high-quality PbS QDs.The method recovers PbCl_(2)with a production ratio of 97%and a purity of 99.99%.PbS QDs and photodetectors synthesized from recycled PbCl_(2)(R-PbCl_(2))have comparable performance and quality to those made using commercial PbCl_(2).R-PbCl_(2)-derived photodetectors exhibit a high external quantum efficiency of 49.6%and a high specific detectivity of 6.95×10^(12)Jones compared to published studies.Additionally,based on R-PbCl_(2),a PbS QD image sensor with 640×512 resolution successfully discriminated common solvents.Moreover,through life-cycle assessment and economic cost analysis,this novel synthesis route offers great advantages in the environmentally friendly use of chemical reagents and reduces the production cost of PbS QDs by 23.2%compared to commercial PbCl_(2).Thus,this work not only contributes to the green recycling of spent lead paste but also provides a low-cost strategy for synthesizing PbS QDs and their optoelectronic application.
基金supported by the National Key Research and Development Program of China(No.2021YFA0715502)the National Natural Science Foundation of China(No.62475084)+2 种基金the Scientific Research Project of Wenzhou(No.G2023025)the Innovation Project of Optics Valley Laboratory(No.OVL2023ZD002)the Fund from Science,Technology and Innovation Commission of Shenzhen Municipality(No.GJHZ20220913143403007).
文摘The bulky footprint of near-infrared(NIR)spectrometers has been limiting their applications in portable and movable systems for probing molecular compositions and structures.Quantum dot(QD)computational spectrometers are a promising strategy for miniaturized NIR spectrometers,whose performance is limited by the poor spectral encoding matrix and,ultimately,the poor quality of PbS QDs.Here,we show that the monodispersity and finely controlled absorption peak of PbS QDs are critical parameters affecting the spectral resolution and noise resistance.Thus,a facile synthesis of a series of monodisperse PbS QDs from a single batch is developed using cation exchange synthesis in a seeded-growth manner.All the as-synthesized PbS QDs have narrow size distributions of below 4%,and the peak intervals can be controlled to within 3 nm.Furthermore,stable PbS QD inks are prepared by considering the compatibility between QD ligands,solvents,and polymers.The PbS QD filter array is fabricated using a contact printing method,exhibiting supreme transmittance curves and a spectral encoding matrix.The filter array is coupled with an InGaAs image sensor to form the QD NIR computational spectrometer.Thanks to the high-quality PbS QDs,the QD spectrometer shows a high spectral resolution of 1.5 nm in a broad wavelength range of 900−1700 nm and excellent spectral reconstruction of narrow and broad spectra with fidelities of above 0.987.Additionally,the QD spectrometer is applied to distinguish materials and accurately measure the alcohol content of white wines,demonstrating the great potential for practical applications of QD NIR spectrometers.
基金supported by the National Key Research and Development Program of China(No.2022YFB3602902)Zhejiang Provincial Natural Science Foundation of China(No.LR21F050001)+5 种基金YONGJIANG Talent Introduction Program(No.2021A-038-B)Ningbo 3315 Program(No.2020A01-B)Zhejiang Innovation and Entrepreneurship Team(No.2021R01003)Science and Technology Innovation 2025 Major Project of Ningbo(No.2022Z085)supported by the Flexible Electronics Zhejiang Province Key Laboratory fund project(No.2022FE002)and the Key projects of National Natural Science Foundation of China(No.62234004)dedicated in memory of Dr.Lei Qian,who was a great mentor,colleague,and friend.He made many significant scientific contributions during his highly productive career and will be remembered.
文摘Stability under light is critical for lead sulfide quantum dots(PbS QDs)in solar cell applications.To improve the stability of PbS QDs solar cells,the influence of the light illumination on the performance of the as-prepared PbS QDs solar cells was carefully investigated.Combined with X-ray and ultraviolet photoelectron spectroscopies,it was revealed that the 1,2-ethanedithiol(EDT)ligands of the hole transport p-type PbS QDs reacted with the ligands of the PbS QDs active layer under light illumination.The reaction not only undermines the n-type characteristics of the active layer,but also increases the number of defects,leading to a serious deterioration in device performance.An interface layer was introduced to block the EDT penetration to avoid this issue,significantly improving the stability of the device under light irradiation.Moreover,the separation of carriers was also enhanced due to the better matching the energy level of the interface layer.The device with an interface layer yielded a power conversion efficiency of 12.55%and sustained to a long time light illumination.
