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| 1 | Electroactive polymeric nanofibrous composite to drive in situ construction of lithiophilic SEI for stable lithium metal anodes显示文摘Uncontrolled lithium dendrite growth hinders the practical application of lithium metal batteries(LMBs).Herein,we report a novel Li^(+) flux distributor achieved by placing an electroactive polyvinylidene fluoride/polymethyl methacrylate(PVDF/PMMA)composite nanofiber interlayer on a current collector,inducing uniform lithium deposition to mitigate the dendrite problem.Specifically,the released PMMA reacts with Liþto form abundant C–O–Li bonds and generate in situ a stable lithiophilic PMMA-Li solid electrolyte interphase layer.Theoretical calculations reveal that polar C–F groups in the PVDF framework and lithiophilic PMMA-Li provide homo-dispersed Li^(+) migration pathways with low energy barriers.Consequently,uniform Li nucleation is achieved at the molecular level,resulting in ultrahigh cycling stability with dendrite-free Li deposition at 5 mA cm^(-2) and 5 mAh cm^(-2)for over 500 h.The PVDF/PMMA||Li||LiFePO_(4)(LFP)full cell presents an increased rate capacity of 110 mAh g^(-1) at 10 C.In addition,a soft-package battery demonstrates a high energy density of 289 Wh kg^(-1).This work provides a facile design for stable lithium metal anodes to promote the practical use of LMBs and other alkali metal batteries. | Ai-Long Chen Nan Shang Yue Ouyang Lulu Mo Chunyang Zhou Weng Weei Tjiu Feili Lai Yue-E Miao Tianxi Liu | 2022 | eScience2022，2，2： | 3 |
| 2 | Structural engineering of cathodes for improved Zn-ion batteries显示文摘Aqueous zinc-ion batteries(ZIBs) are attracting considerable attention because of their low cost,high safety and abundant anode material resources.However,the major challenge faced by aqueous ZIBs is the lack of stable and high capacity cathode materials due to their complicated reaction mechanism and slow Zn-ion transport kinetics.This study reports a unique 3 D ’flower-like’ zinc cobaltite(ZnCo_(2)O_(4-x)) with enriched oxygen vacancies as a new cathode material for aqueous ZIBs.Computational calculations reveal that the presence of oxygen vacancies significantly enhances the electronic conductivity and accelerates Zn^(2+) diffusion by providing enlarged channels.The as-fabricated batteries present an impressive specific capacity of 148.3 mAh g^(-1) at the current density of 0.05 A g^(-1),high energy(2.8 Wh kg^(-1)) and power densities(27.2 W kg^(-1)) based on the whole device,which outperform most of the reported aqueous ZIBs.Moreover,a flexible solid-state pouch cell was demonstrated,which delivers an extremely stable capacity under bending states.This work demonstrates that the performance of Zn-ion storage can be effectively enhanced by tailoring the atomic structure of cathode materials,guiding the development of low-cost and eco-friendly energy storage materials. | Jiajia Huang Yuying Li Ruikuan Xie Jianwei Li Zhihong Tian Guoliang Chai Yanwu Zhang Feili Lai Guanjie He Chuntai Liu Tianxi Liu Dan J.L.Brett | 2021 | Journal of Energy Chemistry2021，30，7： | 3 |
| 3 | Non-metallic electronic regulation in CuCo oxy-/thio-spinel as advanced oxygen evolution electrocatalysts显示文摘Developing cost-effective and high-performance oxygen evolution reaction(OER)electrocatalysts has become the intense research on pursuing emerging renewable energy conversion,in which exploring and investigating the intrinsic nature of efficient and stable Cu Co spinel catalysts toward OER in alkaline media is highly desirable.Herein,Cu1–xCo2+xO4oxy-spinel nanoflakes are fabricated by a facile hydrothermal method with the oxidation of ammonia water.In the same condition,Cu1–xCo2+xS4thio-spinel nanospheres are formed without oxidation.In OER process,the as-obtained Cu1–xCo2+xO4nanoflakes and Cu1–xCo2+xS4nanospheres possess the anodic overpotential of 267 and 297 m V in alkaline media to drive the current density of 10 m A/cm^2,respectively,outperforming the state-of-the-art noble metal catalyst of RuO2.X-ray photoelectron spectroscopy analysis exhibits the higher ratio value of Co(Ⅲ)/Co(Ⅱ)in Cu1–xCo2+xO4than that in Cu1–xCo2+xS4,suggesting that the stronglyelectronegative oxygen efficiently predominates in regulating valence states of Co active sites in spinel structures.Remarkably,density functional theory simulation further reveals that the increased valence state of Co could accelerate the electron exchange between catalysts and oxygen adsorbates during electrocatalysis,thus contributing to the higher OER activity of Cu1–xCo2+xO4catalysts.This work provides deep insight regarding the significance of non-metal element(O and S)in Cu Co spinel structure catalysts,as well as presents a promising approach to exploit higher performance and grasp the mechanism of various non-noblemetal spinel catalysts for water oxidation. | Huan Yang Shuai Gao Dewei Rao Chaonan Zhang Xuecheng Zhou Shaokang Yang Jingjing Ye Shasha Yang Feili Lai Xiaohong Yan | 2021 | Science China Chemistry2021，64，1： | 1 |
| 4 | Visualizing light-induced dynamic structural transformations of Au clusters-based photocatalyst via in situ TEM显示文摘Ultrasmall gold(Au)clusters have been regarded as one of the prototypes materials for solar energy conversion due to their unique strong molecular-like light absorption properties.However,the light-induced aggregation of Au clusters into nanoparticles is one of the most important factors that restricts its application in photocatalysis.Although Au clusters aggregation has been widely demonstrated,the underlying mechanism for cluster fusion is still unclear due to the lack of experimental evidence.Herein,we report the direct observation of Au clusters on TiO_(2) nanosheets aggregating when used as visible light photocatalysts for the reduction of nitroaromatics.Through in situ high-resolution transmission electron microscopy(TEM),the coexistence of two fusion mechanisms of Au clusters on TiO_(2) under ultraviolet-visible(UV-Vis)light irradiation in air is identified,i.e.,the migration and coalescence(MC)and Ostwald ripening(OR).Additionally,the correlation between the photostability of Au clusters and reaction atmospheres has been investigated,among which Au clusters have higher stability in an inert N_(2) atmosphere or vacuum than the oxidizing atmospheres(i.e.,air and O_(2)).These results indicate the inherent stability of Au cluster during photocatalysis,and instability comes from the consuming of ligand layer.This work not only discloses the underlying mechanism of Au cluster sintering but also provides guidelines for enhancing metal clusters-based photocatalysts stability. | Bo Weng Youhong Jiang Hong-Gang Liao Maarten B.J.Roeffaers Feili Lai Haowei Huang Zichao Tang | 2021 | Nano Research2021，14，8： | 1 |
| 5 | Modulating Pd e_(g) orbital occupancy in Pd-Au metallic aerogels for efficient carbon dioxide reduction显示文摘The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the orbitals.Herein,we present a new strategy to modulate the e_(g) orbital occupancy of Pd by constructing composition-controllable Pd-Au metallic aerogels(MAs),optimizing the d-band center of Pd to achieve excellent performance for electrochemical carbon dioxide reduction reaction(CO_(2)RR).Specifically,Pd_(1)Au_(2) MAs achieve almost 100% Faraday efficiency(FE) of CO in the range of-0.40 to-0.80 V vs.reversible hydrogen electrode(RHE),as well as the long-term stability,being one of the best Pd-based materials for CO_(2)RR.The X-ray photoelectron spectroscopy(XPS) results and density functional theory(DFT) calculations demonstrate that the introduction of Au modulates the Pd e_(g) orbital occupancy,which significantly weakens *CO adsorption on Pd,reduces the CO_(2)RR energy barrier and consequently improves the electrocatalytic activity and stability for long-term applications.Our work highlights a new strategy for designing efficient electrocatalysts for CO_(2)RR and beyond. | Yao Chen Juan Wang Tingjie Mao Cun Chen Hanjun Li Honggang Huang Hui Fu Feili Lai Jiadong Chen Nan Zhang Tianxi Liu | 2023 | Journal of Energy Chemistry2023，，12： | 0 |
| 6 | Bimetallic NiCo boride nanoparticles confined in a MXene network enable efficient ambient ammonia electrosynthesis显示文摘Ambient electrocatalytic nitrogen fixation is an emerging technology for green ammonia synthesis,but the absence of optimized,stable and performant catalysts can render its practical application challenging.Herein,bimetallic NiCo boride nanoparticles confined in MXene are shown to accomplish highperformance nitrogen reduction electrolysis.Ta king advantage of the synergistic effect in specific compositions with unique electronic d and p orbits and typical architecture of rich nanosized particles embedded in the interconnected conductive network,the synthesized MXene@NiCoB composite demonstrates extensive improvements in nitrogen molecule chemisorption,active area exposure and charge transport.As a result,optimal NH3 yield rate of 38.7μg h^(-1) mgcat^(-1).and Faradaic efficiency of 6.92%are acquired in0.1 M Na_(2)SO_(4) electrolyte.Moreover,the great catalytic performance can be almost entirely maintained in the cases of repeatedly-cycled and long-term electrolysis.Theoretical investigations reveal that the nitrogen reduction reaction on MXene@NiCoB catalyst proceeds according to the distal pathway,with a distinctly-reduced energy barrier relative to the Co2B counterpart.This work may inspire a new route towards the rational catalyst design for the nitrogen reduction reaction. | Chuang Wang Qin-Chao Wang Ke-Xin Wang Michiel De Ras Kaibin Chu Liang-Liang Gu Feili Lai Sheng-You Qiu Hele Guo Peng-Jian Zuo Johan Hofkens Xiao-Dong Zhu | 2023 | Journal of Energy Chemistry2023，，2： | 0 |
| 7 | d-d Orbital coupling induced by crystal-phase engineering assists acetonitrile electroreduction to ethylamine显示文摘The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation. | Honggang Huang Yao Chen Hui Fu Cun Chen Hanjun Li Zhe Zhang Feili Lai Shuxing Bai Nan Zhang Tianxi Liu | 2024 | Journal of Energy Chemistry2024，89，2： | 0 |
| 8 | Engineering versatile Au-based catalysts for solar-to-fuel conversion显示文摘Gold(Au) nanostructures(NSs) have been widely employed as cocatalysts to improve the photoactivity of semiconductor materials, while a systematic summary of the engineering approaches of Au NSs to maximize the solar-to-fuel conversion efficiency is still lacking. In this review, the recently developed strategies for elevating the overall photocatalytic performance of Au-based catalysts and the deep physical chemistry mechanisms are highlighted. Firstly, the synthetic approaches of Au NSs are summarized, followed by an elaboration on their multiple functions in improving photoactivity. Afterward, modification strategies of Au NSs used to enhance the photocatalytic efficiency of Au-semiconductor composites,including controlling the Au NSs morphology, size, crystal phase, defect engineering, alloying with different metals, modulating interfacial interaction, and introducing an external field, are summarized and discussed independently. Additionally, advanced characterization techniques that can provide insights into the charge dynamics of the photocatalysts are introduced. Finally, we share our opinion on the challenges and outline potentially promising opportunities and directions for efficient Au-based photocatalysis research moving forward. We sincerely look forward to this review can deliver insightful views to design efficient Au-based photocatalysts and spur certain innovations to other metal-based catalysts. | Chunhua Wang Hongwen Zhang Feili Lai Zhirun Xie Yun Hau Ng Bo Weng Xuejiao Wu Yuhe Liao | 2023 | Journal of Energy Chemistry2023，，8： | 0 |
| 9 | Visible light-driven superoxide generation by conjugated polymers for organic synthesis显示文摘得益于他们的唯一的去除的电子结构,结合的基于聚合物的半导体广泛地在器官的电子学,传感器,和生物医学的应用的地里被使用。然而,因为,结合的聚合物的 photocatalytic 性质很少被学习了他们的不合适乐队结构。此处,我们有创作力地证明乐队结合的聚合物组织,提供为有悦耳的轻吸收性质的没有金属的光催化剂的设计的有效策略是强烈与他们聚合(DP ) 的度有关。poly 拿(3- hexylthiophene )(PHT ) 作为一个例子,我们证明有合适的 DP 的 PHT nanofibers 是新奇可见光驱动的光催化剂,它能乐意地把分子的氧变换成 superoxide 离子。得益于产生 superoxides 的高选择, PHT nanofibers 显示为进 imines 与的胺的氧气的氧化的突出的活动将近百分之百变换和选择。这研究为先进结合的基于聚合物的光催化剂的设计提供新策略。 | Feili Lai Yue Wang Dandan Li Xianshun Sun Juan Peng Xiaodong Zhang Yupeng Tian Tianxi Liu | 2018 | Nano Research2018，11，2： | 0 |
| 10 | Interface-induced polymerization strategy for constructing titanium dioxide embedded carbon porous framework with enhanced chemical immobilization towards lithium polysulfides显示文摘The shuttle effect induced by soluble lithium polysulfides(LiPSs)is known as one of the crucial issues that limit the practical applications of lithium-sulfur(Li-S)batteries.Herein,a titanium dioxide nanoparticle embedded in nitrogen-doped porous carbon nanofiber(TiO_(2)@NCNF)composite is constructed via an interface-induced polymerization strategy to serve as an ideal sulfur host.Under the protection of the nanofiber walls,the uniformly dispersed TiO_(2) nanocrystalline can act as capturing centers to constantly immobilize LiPSs towards durable sulfur chemistry.Besides,the mesoporous microstructure in the fibrous framework endows the TiO_(2)@NCNF host with strong physical reservation for sulfur and LiPSs,sufficient pathways for electron/ion transfer,and excellent endurance for volume change.As expected,the sulfur-loaded TiO_(2)@NCNF composite electrode presents a fabulous rate performance and long cycle lifespan(capacity fading rate of 0.062%per cycle over 500 cycles)at 2.0 C.Furthermore,the assembled Li-S batteries harvest superb areal capacity and cycling stability even under high sulfur loading and lean electrolyte conditions. | Yue Ouyang Xiaoxiao Li Jiexin Zhu Wei Zong Yuhang Dai Xuan Gao Wei Zhang Shengyuan Yang Roohollah Bagherzadeh Feili Lai Yue-E Miao Tianxi Liu | 2024 | Nano Research2024，17，3： | 0 |
| 11 | Mo/Fe bimetallic pyrophosphates derived from Prussian blue analogues for rapid electrocatalytic oxygen evolution显示文摘Efficient and stable oxygen evolution electrocatalysts are indispensable for industrial applications of water splitting and hydrogen production.Herein,a simple and practical method was applied to fabricate(Mo,Fe)P2O7@NF electrocatalyst by directly growing Mo/Fe bimetallic pyrophosphate derived from Prussian blue analogues on three-dimensional porous current collector.In alkaline media,the developed material possesses good hydrophilic features and exhibits best-in-class oxygen evolution reaction(OER)performances.Surprisingly,the(Mo,Fe)P_(2)O_(7)@NF only requires overpotentials of 250 and 290 mV to deliver 100 and 600 mA cm^(-2)in 1 mol L^(-1)KOH,respectively.Furthermore,the(Mo,Fe)P_(2)O_(7)@NF shows outstanding performances in alkaline salty water and 1 mol L^(-1)high purity KOH.A worthwhile pathway is provided to combine bimetallic pyrophosphate with commercial Ni foam to form robust electrocatalysts for stable electrocatalytic OER,which has a positive impact on both hydrogen energy application and environmental restoration. | Jingyi Wang Jiajia Huang Siyu Zhao Ivan PParkin Zhihong Tian Feili Lai Tianxi Liu Guanjie He | 2023 | Green Energy & Environment2023，8，5： | 0 |
| 12 | First-principle calculation of distorted T-carbon as a promising anode for Li-ion batteries with enhanced capacity, reversibility, and ion migration properties显示文摘Carbon group element-based materials are the most widely used anode materials for Li-ion batteries(LIBs).However,their performance is limited by the low capacity(eg,graphite)or high-volume changes(eg,Si and Sn).Therefore,exploring high-performance anode materials is quite appealing and promising.By first-principle calculations in this study,we found that distorted T-carbon(DTC)as a desired LIB anode shows properties of the enhanced capacity,decreased volume change,and the increased ion migration.The origin of such improved properties is attributed to the interconnected tunnels and large cavities of the carbon skeleton.The theoretical specific capacity of DTC is found to be 558 mAh/g,which is 1.5 times higher than that of commercial graphite anodes.Interestingly,the volume change of the DTC anode is only 3%at the full-lithiation state(one-fifth of that of the commercial graphite anode),which can overcome the pulverization problem in most high-capacity anode materials and attain a longer cycling lifetime.Both transition state calculations and molecular dynamics simulations demonstrate that the Li-ion migration barrier is less than 0.1 eV and the Li-ion vacancy is only 0.2 eV,enabling its promising rate performance.This study provides a new and effective strategy to improve the anode properties of LIBs. | Jianrui Feng Chao Yang Lijie Zhang Feili Lai Lei Du Xiaohua Yang | 2020 | Carbon Energy2020，2，4： | 0 |
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