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Accelerating directional charge separation via built-in interfacial electric fields originating from work-function differences

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Chinese Journal of Catalysis 2021年第4期42卷 583-594页

作者： Chao Xue Hua An Guosheng Shao Guidong Yang state centre for international cooperation on designer low-carbon and environmental materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001HenanChina XJTU-Oxford international Joint Laboratory for Catalysis School of Chemical Engineering and TechnologyXi'an Jiaotong UniversityXi'an 710049ShaanxiChina

In this work,a hierarchical porous SnS_(2)/rGO/TiO_(2)hollow sphere heterojunction that allows highly-efficient light utilization and shortening distance of charge transformation is rationally designed and *** importantly,an rGO interlayer is successfully embedded between the TiO_(2)hollow sphere shells and outermost SnS_(2)*** interlayer functions as a bridge to connect the two light-harvesting semiconductors and acts as a hole injection layer in the tandem *** induced built-in electric fields on both sides of the interface precisely regulate the spatial separation and directional migration of the photo-generated holes from the light-harvesting semiconductor to the rGO hole injection *** synergistic effects greatly prolong the lifetime of the photo-induced charge *** optimized tandem heterojunction with a 2 wt%rGO loading demonstrate enhanced visible-light-driven photocatalytic activity for Rhodamine B(RhB)dye degradation(removal rate:97.3%)and Cr(VI)reduction(removal rate:97.09%).This work reveals a new strategy for the rational design and assembly of hollow-structured photocatalytic materials with spatially separated reduction and oxidation surfaces to achieve excellent photocatalytic performance.

关键词： SnS_(2)/rGO/TiO_(2) Hollow sphere Photocatalyst Hole injection layer Cr(VI)reduction

Enabling Argyrodite Sulfides as Superb Solid-state Electrolyte with Remarkable Interfacial Stability Against Electrodes

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Energy & environmental materials 2022年第3期5卷 852-864页

作者： Hongjie Xu Guoqin Cao Yonglong Shen Yuran Yu Junhua Hu Zhuo Wang Guosheng Shao School of materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China state centre for international cooperation on designer low-carbon&environmental materials(CDLCEM) Zhengzhou UniversityZhengzhou 450001China Zhengzhou materials Genome Institute(ZMGI) Building 2Zhongyuanzhigu Xingyang 450100China

While argyrodite sulfides are getting more and more attention as highly promising solid-state electrolytes(SSEs)for solid batteries,they also suffer from the typical sulfide setbacks such as poor electrochemical compatibility with Li anode and high-voltage cathodes and serious sensitivity to humid air,which hinders their practical ***,we have devised an effective strategy to overcome these challenging shortcomings through modification of chalcogen chemistry under the guidance of theoretical *** resultant Li_(6.25)PS_(4)O_(1.25)Cl_(0.75)delivered excellent electrochemical compatibility with both pure Li anode and high-voltage LiCoO_(2)cathode,without compromising the superb ionic conductivity of the pristine ***,the current SSE also exhibited highly improved stability to oxygen and humidity,with further advantage being more insulating to *** remarkably enhanced compatibility with electrodes is attributed to in situ formation of helpful electrolyte–electrode *** formation of in situ anode–electrolyte interphase(AEI)enabled stable Li plating/stripping in the Li|Li_(6.25)PS_(4)O_(1.25)Cl_(0.75)|Li symmetric cells at a high current density up to 1 mA cm^(-2)over 200 h and 2 mA cm^(-2)for another 100 *** in situ amorphous nano-film cathode–electrolyte interphase(CEI)facilitated protection of the SSE from decomposition at elevated ***,the synergistic effect of AEI and CEI helped the LiCoO_(2)|Li_(6.25)PS_(4)O_(1.25)Cl_(0.75)|Li full-battery cell to achieve markedly better cycling stability than that using the pristine Li_(6)PS_(5)Cl as SSE,at a high area loading of the active cathode material(4 mg cm^(-2))in type-2032 coin *** work is to add a desirable SSE in the argyrodite sulfide family,so that high-performance solid battery cells could be fabricated without the usual need of strict control of the ambient atmosphere.

关键词： al oying chemistry argyrodite sulfide compatibility with high-voltage cathode and lithium anode fast solid lithium ion conductor resilience to humid air

Tailoring organic bulk-heterojunction for charge extraction and spectral absorption in CsPbBr perovskite solar cells

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Science China materials 2021年第4期64卷 798-807页

作者： Jian Du Jialong Duan Yanyan Duan Qunwei Tang Institute of New Energy Technology College of Information Science and TechnologyJinan UniversityGuangzhou 510632China state centre for international cooperation on designer low-carbon and environmental Material(SCICDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China

All-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising candidates to balance the stability and efficiency issues of organic-inorganic hybrid ***,the large energy barrier for charge transfer and narrow spectral response are still two challenging problems for performance *** present here an organic bulkheterojunction{poly(3-hexylthiophene-2,5-diyl):[6,6]-phenyl C61 butyric acid methyl ester(P3HT:PCBM)}photoactive layer to boost the charge extraction and to widen the spectral absorption,achieving an enhanced power conversion efficiency up to 8.94%by optimizing the thickness of P3HT:PCBM photoactive layer,which is much higher than 6.28%for the pristine CsPbBr_(3)*** interaction between the carbonyl group in PCBM and unsaturated Pb atom in the perovskite surface can effectively passivate the defects and reduce charge ***,the coupling effect between PCBM and P3HT widens the spectral response from 540 to 650 nm for an increased short-circuit current *** importantly,the devices are relatively stable over 75 days upon persistent attack by 70%relative humidity in air *** advantages of high efficiency,excellent long-term stability,cost-effectiveness and scalability may promote the commercialization of inorganic PSCs.

关键词： inorganic CsPbBr3 perovskite solar cells bulk-heterojunction charge extraction spectral absorption stability

Stable all-solid-state battery enabled with Li_(6.25)PS_(5.25)Cl_(0.75) as fast ion-conducting electrolyte

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Journal of Energy Chemistry 2021年第2期30卷 147-154,I0006页

作者： Weidong Xiao Hongjie Xu Minjie Xuan Zhiheng Wu Yongshang Zhang Xiangdan Zhang Shijie Zhang Yonglong Shen Guosheng Shao School of materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina centre for international cooperation on designer low-carbon environmental materials(CDLCEM) Zhengzhou UniversityZhengzhou 450001HenanChina Zhengzhou materials Genome Institute(ZMGI) Zhengzhou 450100HenanChina

All-solid-state batteries(ASSB) with lithium anode have attracted ever-increasing attention towards developing safer batteries with high energy *** great advancement has been achieved in developing solid electrolytes(SE) with superb ionic conductivity rivalling that of the current liquid technology,it has yet been very difficult in their successful application to ASSBs with sustaining rate and cyclic *** in this work,we have realized a stable ASSB using the Li_(6.25)PS_(5.25)Cl_(0.75) fast ionconducting electrolyte together with LiNbO_3 coated LiCoO_2 as cathode and lithium foil as the *** effective diffusion coefficient of Li-ions in the battery is higher than 10^(-12) cm~2 s^(-1),and the significantly enhanced electrochemical matching at the cathode-electrolyte interface was essential to enable long-term stability against high oxidation potential,with the LCO@LNO/Li_(6.25)PS_(5.25)Cl_(0.75)/Li battery to retain 74.12% capacity after 430 cycles at 100 μA cm-2 and 59.7% of capacity after 800 cycles at 50 μA cm^(-2),at a high charging cut-off voltage of 4.2 *** demonstrates that the Li_(6.25)PS_(5.25)Cl_(0.75) can be an excellent electrolyte for the realization of stable ASSBs with high-voltage cathodes and metallic lithium as anode,once the electrochemical compatibility between cathode and electrolyte can be addressed with a suitable buffer coating.

关键词： All-solid-state batteries Sulfide electrolyte Li_(6.25)PS_(5.25)Cl_(0.75) LiNbO_(3)coating Lithium anode Long-term stability

Coupling effect of the conductivities of Li ions and electrons by introducing LLTO@C fibers in the LiNi0.8Co0.15Al0.05O2 cathode

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international Journal of Minerals,Metallurgy and materials 2021年第2期28卷 305-316页

作者： Hao-yang Wang Xue Cheng Xiao-feng Li Ji-min Pan Jun-hua Hu School of materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China state Center for international cooperation on designer low-carbon&environmental materials(CDLCEM) Zhengzhou UniversityZhengzhou 450001China Zhengzhou materials Genome Institute(ZMGI) Xingyang 450100China

To probe the coupling effect of the electron and Li ion conductivities in Ni-rich layered materials(LiNi0.8Co0.15Al0.05O2,NCA),lithium lanthanum titanate(LLTO)nanofiber and carbon-coated LLTO fiber(LLTO@C)materials were introduced to polyvinylidene difluoride in a *** enhancement of the conductivity was indicated by the suppressed impedance and *** 1 and 5 C,the cathodes with coupling conductive paths had a more stable cycling *** coupling mechanism was analyzed based on the chemical state and structure evolution of NCA after cycling for 200 cycles at 5 *** the pristine cathode,the propagation of lattice damaged regions,which consist of high-density edge-dislocation walls,destroyed the bulk integrity of *** addition,the formation of a rock-salt phase on the surface of NCA caused a capacity *** contrast,in the LLTO@C modified cathode,although the formation of dislocation-driven atomic lattice broken regions and cation mixing occurred,they were limited to a scale of several atoms,which retarded the generation of the rock-salt phase and resulted in a pre-eminent capacity *** NiO phase“pitting”occurred.A mechanism based on the synergistic transport of Li ions and electrons was proposed.

关键词： Ni-rich cathode coupling mechanism dislocation wall coaxial structure cation mixing

Samarium doping improves luminescence efficiency of Cs_(3)Bi_(2)Br_(g)perovskite quantum dots enabling efficient white light-emitting diodes

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Journal of Rare Earths 2021年第4期39卷 374-379页

作者： Yongsheng Zhu Jinyang Zhu Haizhen Song Jinshu Huang Zhiwen Lu Gencai Pan College of Physics and Electronic Engineering Nanyang Normal UniversityNanyang 473061China state centre for international cooperation on designer low-carbon&environmental materials School of Materials Science and EngineeringZhengzhou University Zhengzhou 450001ChinaSchool of Physics and ElectronicsHenan UniversityKaifeng 475004China

Considering the toxicity problem of lead-based perovskite quantum dots(PQDs),the lead-free Cs_(3)Bi_(2)Br_(g)PQDs has been recognized as one of the promising ***,the low photoluminescence quantum yields(PLQYs)hinder its practical application in optoelectronic ***,w e successfully prepared Sm^(3+)ions doped Cs_(3)Bi_(2)Br_(g)PQDs with effective white light-emission by modified ligandassisted recrystallization *** realization of white light-emission is attributed to the broadband blue emission of excitons and the red emission(^(4)G_(5/2)-^(6)HJ(J=5/2,7/2,9/2))of Sm^(3+)ions for Sm^(3+)ions doped Cs_(3)Bi_(2)Br_(g)*** importantly,compared with the undoped Cs_(3)Bi_(2)Br_(g)PQDs,the PLQYs of Sm^(3+)ions doped Cs_(3)Bi_(2)Br_(g)PQDs are improved from 10.9%to 20.8%,and the anti-water stability is also obviously ***,the Sm^(3+)ions doped PQDs based white light-emitting diodes(LEDs)with luminous efficiency of 12.6 lm/W were explored,which indicates that there is a potential prospect of lead-free PQDs in white light lighting application.

关键词： Lead-free perovskite quantum dots Photoluminescence quantum yields Energy transfer White light-emitting diodes Rare earths

Bio-inspired construction of electrocatalyst decorated hierarchical porous carbon nanoreactors with enhanced mass transfer ability towards rapid polysulfide redox reactions

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Nano Research 2021年第11期14卷 3942-3951页

作者： Shijie Zhang Yongshang Zhang Guosheng Shao Peng Zhang School of materials Science and Engineering Zhengzhou UniversityZhengzhou450001China state centre for international cooperation on designer low-carbon&environmental materials(CDLCEM) Zhengzhou University100 Kexue AvenueZhengzhou450001China Zhengzhou materials Genome Institute Building 2ZhongyuanzhiguXingyang450100China

Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth process of lithium sulfide leads to a thick insulating film covering the electrode, inducing slow electrons transfer and mass-transfer of ions and liquid sulfur species in working Li-S cells. Here, we demonstrate a bio-inspired strategy of constructing ant-nest-like hierarchical porous ultrathin carbon nanosheet networks with the implants of metallic nanoparticles electrocatalysts (HPC-MEC) as efficient nanoreactors enabling rapid mass transfer, via a simple and green NaCl template. Such nanoreactors with a large active surface area could effectively anchor polysulfides for mitigating the shuttle effect, facilitating uniformly thin Li2S film, and promoting the mass transfer for fast sulfur species conversions. This helps contribute to a continuously high sulfur utilization in Li-S batteries with the HPC-MEC reactors. As a typical exhibition, cobalt embedded hierarchical porous carbon (HPC-Co) could realize to deliver a remarkably high specific capacity of 1,540.6 mAh·g−1, an excellent rate performance of 878.8 mAh·g−1 at 2 C, and high area capacity of 11.6 mAh·cm−2 at a high sulfur load of 10 mg·cm−2 and low electrolyte/sulfur ratio of 5 µL·mg−1.

关键词： sulfur species reactor hierarchical porous carbon network electrocatalyst high sulfur loading low electrolyte/sulfur ratio

Recent Advances in Effective Reduction of Graphene Oxide for Highly Improved Performance Toward Electrochemical Energy Storage

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Energy & environmental materials 2018年第1期1卷 5-12页

作者： Peng Zhang Zhi Li Shijie Zhang Guosheng Shao School of materials Science and Engineering Zhengzhou UniversityZhengzhou450001China state centre for international cooperation on designer low-carbon&environmental materials(CDLCEM) Zhengzhou UniversityZhengzhou450001Henan China Zhengzhou materials Genome Institute ZhongyuanzhiguXingyang450100China

The demand for high-quality graphene from various applications promotes the exploration of various synthesis methods such as chemical vapor deposition,chemical reduction of graphite oxide,liquid-phase exfoliation,and electrochemical *** those,chemical treatments for the production of reduced graphene oxide(RGO)dictate the current technologies for mass production of graphene ***,such conventional chemical reduction methods are rather ineffective in removing oxygen-containing functional groups from graphene oxide(GO),with resultant RGO products containing high level of structural *** leads to significantly damaged crystallinity and drastically lowered electric and thermal conductivity,which is probably the main bottleneck to limit the performance of RGO-based *** efforts such as thermal reduction,microwave-irradiation reduction,or other novel reduction methods(e.g.,photoreduction)have been developed to repair defects in RGO *** perspective review is to outline the latest advances toward effective reduction of GO for significantly enhanced *** demonstrate that effectively repaired RGO with large specific surface area and highly improved crystallinity is key to highly improved electric and thermal conductivity,thus leading to significantly enhanced properties essential for chemical energy storage devices.

关键词： materials conductivity removing

Review on engineering two-dimensional nanomaterials for promoting efficiency and stability of perovskite solar cells

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Journal of Energy Chemistry 2022年第5期31卷 154-175页

作者： Qingwei Zhou Jialong Duan Yanyan Duan Qunwei Tang Institute of New Energy Technology College of Information Science and TechnologyJinan UniversityGuangzhou 510632GuangdongChina state centre for international cooperation on designer low-carbon and environmental Material(SCICDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001HenanChina

Perovskite solar cell(PSC) has gradually shown its great superiority in photovoltaic filed to compete commercial solar cells owing to its great advantages, such as high efficiency and low fabrication cost. On the way towards commercialization, great efforts have been achieved by accelerating charge extraction and reducing carrier recombination. Recently, two-dimensional(2 D) layered materials have attracted increasing interests for application in PSCs due to their distinctive chemical and physical properties, such as high carrier mobility and tunable bandgap, which greatly determines the perovskite film growth kinetics, carrier transfer and stability of PSCs. Therefore, with the aim to better understand their recent development and application in PSC, in this review, the emerging 2D materials beyond graphene as charge transport layers, buffer layers and additives in perovskite film for enhancing the efficiency and stability of PSCs are summarized. However, there are still some crucial challenges to be addressed for commercialization. Finally, the challenges and prospects of these 2D nanomaterials for application in PSCs are further proposed for future development.

关键词： Perovskite solar cells 2D materials Interface engineering Charge transfer Stability