bluuebunny/crossref_metadata_2025_split huggingface dataset:
Sustainable Prelithiation Strategy: Enhancing Energy Density and Lifespan with Ultrathin Li‐Mg‐Al Alloy Foil
Authors: Chen Xinlong , Yang Fangzhou , Zhang Can , Wan Wang , Liu Ganxiong , Qu Ge , Wang Zhongheng , Li Sa , Huang Yunhui , Wang Chao 
Published: May 2024

AbstractPrelithiation is a well‐established strategy for enhancing battery energy density. However, traditional prelithiation approaches have primarily addressed compensating for the initial active lithium loss (ALL) while overlooking the ALL during extended cycling. In response, a novel method is introduced by increasing the prelithiation degree and pre‐storing stable LiCx within the anode. This innovation facilitates sustainable lithium replenishment, resulting in a significant improvement in battery cycle life and energy density. Moreover, challenges associated with using pure Li foils to realize this strategy in contact prelithiation are revealed, such as difficulties in thinning to less than 5 µm, and the loss of the electronic pathway during prelithiation, resulting in low lithium utilization rates and numerous residues. Additionally, the significantly accelerated capacity fading caused by these residues, typically emerging after hundreds of cycles, has been overlooked. To overcome these challenges, an ultrathin Li‐Mg‐Al alloy foil is developed with significantly improved mechanical properties and delithiation behavior. During prelithiation, the 96Li2Mg2Al alloy maintains a complete film structure with numerous micropores, avoiding randomly distributed debris. This structure ensures high utilization, unimpeded electronic pathways, and efficient electrolyte filtration. By employing a 5‐µm 96Li2Mg2Al foil for sustainable prelithiation, a substantial improvement in energy density is achieved and tripled the battery's lifespan.
Soft Lattice and Phase Stability of α‐FAPbI3
Authors: Kim Hui‐Seon , Park Nam‐Gyu 
Published: May 2024

AbstractSince the certified power conversion efficiency (PCE) of perovskite solar cells (PSCs) has reached 26.1%, exactly equal to that of crystalline silicon solar cells, a strong demand for ensuring the long‐term stability of PSCs has arisen for commercialization. The intrinsic stability of the perovskite layer must be guaranteed as a top priority to ensure the whole device's stability. Recently, the state‐of‐the‐art PSCs, performing a high PCE, employ α‐FAPbI3 (FA = formamidinium) for the perovskite layer in spite of its metastable tendency to spontaneously transform into its photoinactive polymorph at PSC operating temperature. In this review paper, the intrinsic structural stability of α‐FAPbI3 soft lattice is understood from the thermodynamic point of view, with key parameters to restrain the undesirable phase transition. Besides, reported experimental results are closely examined to find fundamental origins, derive the enhanced phase stability in each experiment, and understand their role in maintaining the lattice structure from the collective perspective.
Perovskite Tandem Solar Cells for Low Earth Orbit Satellite Power Applications
Authors: Yoon Geon Woo , Jo Bonghyun , Boonmongkolras Passarut , Han Gill Sang , Jung Hyun Suk 
Published: May 2024

AbstractThe rapid advancement of next‐generation wireless communication technology based on satellite communication using tens of thousands of low Earth orbit (LEO) satellites requires higher technology for solar energy systems. The perovskite solar cells (PSCs) show great potential as modern space solar cells due to high power, high specific power, high radiation resistance, and low cost compared to conventional space solar cells, such as III‐V and Si solar cells. However, the study of PSCs has been almost focused on terrestrial use for commercialization, thereby a few research for PSCs as space solar cells. This review discusses the current progress and future challenges for the space application of PSCs. To understand the space applications, the extreme space environmental conditions are summarized and their impacts on PSCs. Notably, the two‐terminal (2T) monolithic perovskite‐based tandem solar cells (PTSCs) capable of high performance with high efficiency and specific power are discussed. Finally, the key technology and the perspectives for the future development of PSCs are suggested for practical use as space applications.
In Situ Constructing a TiO2/TiN Heterostructure Modified Carbon Interlayer for Balancing the Surface Adsorption and Conversion of Polysulfides in Li–S Batteries
Authors: Yang Shixun , Jiang Dengbang , Su Qian , Yuan Shixiang , Guo Yi , Duan Kaijiao , Xiang Mingwu , Guo Junming , Bai Wei , Chou Shulei 
Published: May 2024

AbstractSevere shuttle effect and sluggish reaction kinetics caused by lithium‐polysulfides have always been the dominant factor to reduce the actual energy density of lithium–sulfur batteries. It's very important to simultaneously balance the surface adsorption and redox conversion of the lithium‐polysulfides. Herein, a TiO2/TiN heterostructure and in situ N‐doping modified multifunctional carbon interlayer is designed and constructed using a melamine foam as the matrix material at a relatively low temperature and without NH3 atmosphere. Interestingly, TiO2 nano‐particles decorated on the N‐enriched melamine carbon foam can be partially in situ transformed into TiN during pyrolysis process. Based on the support of highly conductive and interconnected carbon skeletons, the N heteroatom and TiO2/TiN show good synergetic adsorption and conversion of the soluble lithium‐polysulfides, whilst boosting the electrochemical performance of lithium–sulfur batteries. Consequently, when used the multifunctional carbon interlayer, the Super P/sulfur cathode based lithium–sulfur battery delivers a high initial discharge capacity of 814 mAh g−1 at a high current rate of 2.0 C and maintain the 548 mAh g−1 after 500 cycles. Even with the high sulfur loading of 7.5 mg cm−2 and low E/S ratio of 4.7 µL mg−1, an acceptable areal capacity of 8.2 mAh cm−2 can be obtained.
Electric Field Redistribution Triggered Surface Adsorption and Mass Transfer to Boost Electrocatalytic Glycerol Upgrading Coupled with Hydrogen Evolution
Authors: Zhao Zhefei , Shen Xinyi , Luo Xingyu , Chen Minhao , Zhang Miduo , Yu Ruopeng , Jin Runtao , Zheng Huajun 
Published: May 2024

AbstractElectrocatalytic glycerol oxidation reaction (GOR) stands out as an economical and prospective technology to replace oxygen evolution reaction for co‐producing high‐valued chemicals and hydrogen (H2). Regulating the adsorption of glycerol (GLY) and hydroxyl (OH) species is of great significance for improving the GOR performance. Herein, a hierarchical p–n heterojunction by combining Co‐metal organic framework (MOF) nanosheets with CuO nanorod arrays (CuO@Co‐MOF) is developed to realize the optimization on GOR. Specifically, CuO@Co‐MOF electrode exhibits superior performance with a conversion of 98.4%, formic acid (FA) selectivity of 87.3%, and Faradaic efficiency (FE) of 98.9%. The flow‐cell system with the bifunctional CuO@Co‐MOF electrode for pairing GOR with the hydrogen evolution reaction (HER) reveals better energy conversion efficiency. Experimental results and theoretical calculations unravel the redistributed electric field by introducing Co‐containing species that contribute to the improved performance, which not only enhances the OH adsorption but also modulates the excessive GLY adsorption of CuO, thus reducing reaction energy barriers of FA desorption. Simultaneously, finite element analysis reveals that the novelty hierarchical structure can increase the concentration of OH− and facilitate the mass transfer of OH− in the solution.
A Selenium‐Containing Polymer Donor Enables 16.9% Efficiency in Non‐Fused Electron Acceptor‐Based Organic Photovoltaic Cells
Authors: Xiao Yang , Yao Huifeng , Wang Jingwen , Zhang Tao , Chen Zhihao , Qiao Jiawei , Yang Ni , Yu Yue , Ren Junzhen , Li Zi , Hao Xiaotao , Hou Jianhui 
Published: May 2024

AbstractOrganic photovoltaic cells (OPVs) based on non‐fused electron acceptors (nfEAs) have exhibited substantial progress in enhancing the power conversion efficiency (PCE). However, controlling the morphology of the donor/acceptor blend remains a significant challenge, making the regulation of film formation kinetics crucial. Here, by designing a new selenium‐containing polymer donor PQSe‐TCl, the pre‐aggregation behavior is modulated and finely tune the resultant morphologies. Compared with its thiophene analogue PBQx‐TCl, PQSe‐TCl exhibits a larger π–π stacking distance and weaker pre‐aggregation performance, leading to a longer film‐formation duration in the fabrication process. Consequently, the PQSe‐TCl:A4T‐16‐based device records an outstanding PCE of 16.9%, which is the highest value for fully nfEA‐based OPVs. This study highlights the importance of regulating the film‐formation kinetics for obtaining high‐efficiency nfEA‐based OPVs.
Surface to Bulk Synergetic Modulation of Nickel‐Rich LiNi0.83Co0.06Mn0.11O2 via a Three‐in‐One Approach for Long‐Cycle Lithium‐Ion Batteries
Authors: Zhang Shuping , Wu Jianyang , Jiang Ning , Sun Hao , Yang Huanfang , Shen Lanyao , Zhou Mingyue , Liu Wen , Zhou Henghui , Zhao Hailei 
Published: May 2024

AbstractNickel‐rich cathode materials have gained popularity in the development of lithium‐ion batteries (LIBs) due to their high energy density, which exceeds 250 Wh kg−1. However, the instability of bulk and surface structures has significantly limited their industrial application. In this study, a three‐in‐one approach to synergistically modulate the structure of LiNi0.83Co0.06Mn0.11O2 (NCM83) from surface to bulk by a phytic acid (PA) coating is proposed. This surface treatment leads to the spontaneous formation of an amorphous lithium phosphates coating layer on the outermost surface, a reconstructed NiO layer at the subsurface, and a gradient P doping in the NCM83 bulk. The resulting hierarchical and multifunctional structure provides a facilitated surface Li‐ion conduction, a NiO‐stabilized subsurface with strong resistance toward side reactions between the electrode and electrolyte, a fast Li ion bulk diffusion endowed by the enlarged LiO6 slab due to the P doping, and an enhanced H2−H3 phase transition reversibility. As a result, the PA‐NCM83 sample exhibits excellent capacity retention with 72.4% after 300 cycles at 1 C within 2.8–4.45 V, and 69.8% after 200 cycles at an elevated temperature of 45 °C. This approach provides a facile and efficient method to stabilize Ni‐rich cathode materials for next‐generation high‐energy LIBs.
Unswitched memory B cell deficiency in children with sickle cell disease and response to pneumococcal polysaccharide vaccine
Authors: Tubman Venée N. , Maysonet Daniel , Estrada Norma , Halder Tripti , Ramos Lindsey , Bhamidipati Sameera , Carisey Alexandre F. , Minard Charles G. , Allen Carl E. 
Published: May 2024

AbstractEarly mortality in sickle cell disease (SCD) is attributed to increased infections due to loss of splenic function. Marginal zone B cells are important for initial opsonization of pathogens and can be absent in spleen histopathology in SCD. The frequency of unswitched memory B cells (UMBC), the circulating correlate of marginal zone B cells, reflects the immunologic function of the spleen. We hypothesized that asplenia in SCD is associated with alterations in the peripheral blood lymphocyte population and explored whether UMBC deficiency was associated with a clinical phenotype. We analyzed B cell subsets and clinical history for 238 children with SCD and 63 controls. The median proportion of UMBCs was lower in children with SCD compared with controls (4.7% vs. 6.6%, p < .001). Naïve B cells were higher in SCD compared with controls (80.6 vs. 76.3%, respectively, p = .02). UMBC frequency declined by 3.4% per year increase in age in SCD (95% CI: 2%, 4.7%, p < .001), but not in controls. A majority of children in all cohorts had an IgM concentration in the normal range for age and there were no differences between groups (p = .13). Subjects developed titers adequate for long‐term protection to fewer serotypes in the polysaccharide vaccine than controls (14.7 vs. 19.4, p < .001). In this cohort, bacteremia was rare and specific clinical complications were not associated with UMBC proportion. In summary, UMBC deficiency occurs in SCD and is associated with age. Future studies should investigate B cell subsets prospectively and identify the mechanism of B cell loss in the spleen.
Giant ab‐Plane Birefringence in Quasi‐1D Fibrous Red Phosphorus
Authors: Chen Wujia , Zhang Bowen , Tao Kezheng , Li Qiang , Sun Jia‐Lin , Yan Qingfeng 
Published: May 2024

AbstractQuasi‐one‐dimensional (quasi‐1D) van der Waals crystal fibrous red phosphorus (RP) exhibits pronounced in‐plane optical anisotropy, positioning it as a potential candidate for polarization‐related micro‐nano devices. Unfortunately, a comprehensive investigation into the complex refractive index of fibrous RP and the structure–activity relationship connecting the distinctive quasi‐1D structure with optical anisotropy is currently deficient. Herein, we have collectively determined the complex refractive index of the fibrous RP flakes within the ab‐plane through Kramers–Kronig (KK) analysis and theoretical calculation. Notably, the maximum birefringence of fibrous RP reaches 0.642@475 nm with an absolute extinction coefficient of only 0.08, superior to the reported traditional optical crystals and the emerging low‐dimensional materials as well. The remarkable birefringence can be attributed to the synergistic influence of the large electronic dipole polarizability, anisotropic electron density distribution and the distortion of stereochemically active lone pair (SCALP). This work demonstrates the potential of fibrous RP for polarization‐sensitive devices, illuminating possibilities to exploit novel giant birefringent crystals based on the structure–activity relationship.
Tuning Ion Mobility in Lithium Argyrodite Solid Electrolytes via Entropy Engineering
Authors: Lin Jing , Schaller Mareen , Indris Sylvio , Baran Volodymyr , Gautam Ajay , Janek Jürgen , Kondrakov Aleksandr , Brezesinski Torsten , Strauss Florian 
Published: May 2024

AbstractThe development of improved solid electrolytes (SEs) plays a crucial role in the advancement of bulk‐type solid‐state battery (SSB) technologies. In recent years, multicomponent or high‐entropy SEs are gaining increased attention for their advantageous charge‐transport and (electro)chemical properties. However, a comprehensive understanding of how configurational entropy affects ionic conductivity is largely lacking. Herein we investigate a series of multication‐substituted lithium argyrodites with the general formula Li6+x[M1aM2bM3cM4d]S5I, with M being P, Si, Ge, and Sb. Structure‐property relationships related to ion mobility are probed using a combination of diffraction techniques, solid‐state nuclear magnetic resonance spectroscopy, and charge‐transport measurements. We present, to the best of our knowledge, the first experimental evidence of a direct correlation between occupational disorder in the cationic host lattice and lithium transport. By controlling the configurational entropy through compositional design, high bulk ionic conductivities up to 18 mS cm−1 at room temperature are achieved for optimized lithium argyrodites. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors via entropy engineering, overcoming compositional limitations for the design of advanced electrolytes and opening up new avenues in the field.
Sono‐Triggered Cascade Lactate Depletion by Semiconducting Polymer Nanoreactors for Cuproptosis‐Immunotherapy of Pancreatic Cancer
Authors: Yu Ningyue , Zhou Jianhui , Ding Mengbin , Li Meng , Peng Shaojun , Li Jingchao 
Published: May 2024

AbstractThe high level of lactate in tumor microenvironment not only promotes tumor development and metastasis, but also induces immune escape, which often leads to failures of various tumor therapy strategies. We here report a sono‐triggered cascade lactate depletion strategy by using semiconducting polymer nanoreactors (SPNLCu) for cancer cuproptosis‐immunotherapy. The SPNLCu mainly contain a semiconducting polymer as sonosensitizer, lactate oxidase (LOx) conjugated via a reactive oxygen species (ROS)‐cleavable linker and chelated Cu2+. Upon ultrasound (US) irradiation, the semiconducting polymer generates singlet oxygen (1O2) to cut ROS‐cleavable linker to allow the release of LOx that catalyzes lactate depletion to produce hydrogen peroxide (H2O2). The Cu2+ will be reduced to Cu+ in tumor microenvironment, which reacts with the produced H2O2 to obtain hydroxyl radical (⋅OH) that further improves LOx release via destroying ROS‐cleavable linkers. As such, sono‐triggered cascade release of LOx achieves effective lactate depletion, thus relieving immunosuppressive roles of lactate. Moreover, the toxic Cu+ induces cuproptosis to cause immunogenic cell death (ICD) for activating antitumor immunological effect. SPNLCu are used to treat both subcutaneous and deep‐tissue orthotopic pancreatic cancer with observably enhanced efficacy in restricting the tumor growths. This study thus provides a precise and effective lactate depletion tactic for cancer therapy.
Regulating Spin Density using TEMPOL Molecules for Enhanced CO2‐to‐Ethylene Conversion by HKUST‐1 Framework Derived Electrocatalysts
Authors: Yin Baipeng , Wang Can , Xie Shijie , Gu Jianmin , Sheng Hua , Wang De‐Xian , Yao Jiannian , Zhang Chuang 
Published: May 2024

AbstractThe selectivity of multicarbon products in the CO2 reduction reaction (CO2RR) depends on the spin alignment of neighboring active sites, which requires a spin catalyst that facilitates electron transfer with antiparallel spins for enhanced C−C coupling. Here, we design a radical‐contained spin catalyst (TEMPOL@HKUST‐1) to enhance CO2‐to‐ethylene conversion, in which spin‐disordered (SDO) and spin‐ordered (SO) phases co‐exist to construct an asymmetric spin configuration of neighboring active sites. The replacement of axially coordinated H2O molecules with TEMPOL radicals introduces spin‐spin interactions among the Cu(II) centers to form localized SO phases within the original H2O‐mediated SDO phases. Therefore, TEMPOL@HKUST‐1 derived catalyst exhibited an approximately two‐fold enhancement in ethylene selectivity during the CO2RR at −1.8 V versus Ag/AgCl compared to pristine HKUST‐1. In situ ATR‐SEIRAS spectra indicate that the spin configuration at asymmetric SO/SDO sites significantly reduces the kinetic barrier for *CO intermediate dimerization toward the ethylene product. The performance of the spin catalyst is further improved by spin alignment under a magnetic field, resulting in a maximum ethylene selectivity of more than 50 %. The exploration of the spin‐polarized kinetics of the CO2RR provides a promising path for the development of novel spin electrocatalysts with superior performance.
Revealing Hydrogen Bond Effect in Rechargeable Aqueous Zinc‐Organic Batteries
Authors: Guo Jun , Du Jia‐Yi , Liu Wan‐Qiang , Huang Gang , Zhang Xin‐Bo 
Published: May 2024

AbstractThe surrounding hydrogen bond (H‐bond) interaction around the active sites plays indispensable functions in enabling the organic electrode materials (OEMs) to fulfill their roles as ion reservoirs in aqueous zinc‐organic batteries (ZOBs). Despite important, there are still no works could fully shed its real effects light on. Herein, quinone‐based small molecules with a H‐bond evolution model has been rationally selected to disclose the regulation and equilibration of H‐bond interaction between OEMs, and OEM and the electrolyte. It has been found that only a suitable H‐bond interaction could make the OEMs fully liberate their potential performance. Accordingly, the 2,5‐diaminocyclohexa‐2,5‐diene‐1,4‐dione (DABQ) with elaborately designed H‐bond structure exhibits a capacity of 193.3 mAh g−1 at a record‐high mass loading of 66.2 mg cm−2 and 100 % capacity retention after 1500 cycles at 5 A g−1. In addition, the DABQ//Zn battery also possesses air‐rechargeable ability by utilizing the chemistry redox of proton. Our results put forward a specific pathway to precise utilization of H‐bond to liberate the performance of OEMs.
BINOL‐Based Chiral Macrocycles and Cages
Authors: Yu Yabing , Hu Yaning , Ning Chengbing , Shi Wudi , Yang Ao , Zhao Yibo , Cao Zhong‐Yan , Xu Youzhi , Du Pingwu 
Published: May 2024

AbstractChirality, a fundamental principle in chemistry, biology, and medicine, is prevalent in nature and in organisms. Chiral molecules, such as DNA, RNA, and proteins, are crucial in biomolecular synthesis, as well as in the development of functional materials. Among these, 1,1′‐binaphthyl‐2,2′‐diol (BINOL) stands out for its stable chiral configuration, versatile functionality, and commercial availability. BINOL is widely employed in asymmetric catalysis and chiral materials. This review mainly focuses on recent research over the past five years concerning the use of BINOL derivatives for constructing chiral macrocycles and cages. Their contributions to chiral luminescence, enantiomeric separation, transmembrane transport, and asymmetric catalysis were examined.
Selective Photoreforming of Waste Plastics into Diesel Olefins via Single Reactive Oxygen Species
Authors: Yue Shuai , Zhao Zhiyong , Zhang Tao , Li Fei , Liu Kewang , Zhan Sihui 
Published: May 2024

AbstractThe accumulation of plastic waste poses a pressing environmental challenge. Catalytic conversion stands out as an ideal approach for plastics upcycling, particularly through solar‐driven plastics photoreforming. However, due to the common effects of multiple reactive oxygen species (ROS), selectively generating high‐value chemicals becomes challenging. In this study, we developed a universal strategy to achieve >85 % selective production of diesel olefins (C15–C28) from polyolefin waste plastics via single ROS. Using tetrakis (4‐carboxyphenyl) porphyrin supramolecular (TCPP) with different central metals as an example to regulate single ROS generation, results show Ni‐TCPP facilitates triplet exciton production, yielding 1O2, while Zn‐TCPP generates ⋅O2− due to its strong built‐in electric field (IEF). 1O2 directly dechlorinates polyvinyl chloride (PVC) due to the electro‐negativity of chlorine atoms and the low dissociation energy of C−Cl bonds, while ⋅O2− promotes direct dehydrogenation of polyethylene (PE) due to the electro‐positivity of hydrogen atoms and the high dissociation energy of C−H bonds. This method is universally applicable to various single ROS systems. Installation experiments further affirm the application potential, achieving the highest diesel olefin production of 76.1 μmol h−1. Such a universally adaptive approach holds promise for addressing the global plastic pollution problem.