bluuebunny/crossref_metadata_2025_split huggingface dataset:
Transient Out‐of‐Equilibrium Nucleic Acid‐Based Dissipative Networks and Their Applications
Authors: Li Zhenzhen , Wang Jianbang , Willner Itamar 
Published: April 2022

AbstractDynamic, dissipative reactions play important roles in biological processes, and emulating such biological processes by artificial circuits and networks is a challenging topic in the area of Systems Chemistry. The present article summarizes efforts to apply the information encoded in the base sequence of nucleic acids to assemble transient, dissipative DNA‐based networks mimicking natural processes. The design principles of the transient nucleic acid‐based systems are introduced. Triggered reaction moduli lead to a transient intermediary constituent recovered to the parent moduli by enzymes, DNAzyme, or light as control units are described. Transient DNA‐based circuitries of enhanced complexities revealing temporal gated or cascaded transformations are demonstrated. Different applications of dynamically triggered transient circuits are introduced, including the temporal aggregation and deaggregation of plasmonic nanoparticles or semiconductor quantum dots and the control over their optical properties, the transient release and uptake of loads by aptamer scaffolds, and the transient reconfiguration of constitutional dynamic networks and the control over emergent catalytic functions. The future perspectives of dissipative nucleic acid‐based networks and their potential future applications are discussed.
Bifunctional Fusion Membrane‐Based Hydrogel Enhances Antitumor Potency of Autologous Cancer Vaccines by Activating Dendritic Cells
Authors: Ke Yaohua , Zhu Junmeng , Chu Yanhong , Cen Lanqi , Fu Yao , Fan Xiangshan , Shao Jingyi , Li Rutian , Yu Lixia , Liu Baorui , Liu Qin 
Published: April 2022

AbstractAutologous tumor cell vaccine is an individualized tumor treatment strategy to elicit tumor‐specific immune responses. However, it is difficult to exert efficacy in “cold” tumors, which lack tumor‐infiltrating T cells and are not sensitive to immunotherapy. Here, a dendritic cells (DCs) activation hydrogel is constructed based on bifunctional fusion membrane nanoparticles (FM‐NPs) composed of autologous tumor cell membranes and Mycobacterium phlei membrane extracts. The FM‐NPs not only provide tumor antigens but also can activate DCs. Afterward, the FM‐NPs are loaded in an injectable alginate hydrogel together with granulocyte‐macrophage colony‐stimulating factor (GM‐CSF). GM‐CSF releases rapidly and recruits DCs to hydrogel, while FM‐NPs retain in hydrogel to continuously interconnected with DCs, enriching mature DCs loaded with tumor antigens. In the 4T1 mouse breast tumor model, this hydrogel promotes the maturation of DCs in tumor‐draining lymph nodes and induces sufficient effector memory T cells that migrate to the tumor microenvironment. This successfully converts the “cold” tumors to “hot”, thus exerting a significant antitumor effect synergized with the PD‐1 antibody. It is also verified the inhibitory effect of FM‐NPs using human gastric cancer organoids. Altogether, these findings demonstrate the application potential for the bifunctional fusion membrane‐based hydrogel as an autologous tumor vaccine by activating DCs.
Direct Plasma‐Enhanced‐Chemical‐Vapor‐Deposition Syntheses of Vertically Oriented Graphene Films on Functional Insulating Substrates for Wide‐Range Applications
Authors: Zhou Fan , Shan Junjie , Cui Lingzhi , Qi Yue , Hu Jingyi , Zhang Yanfeng , Liu Zhongfan 
Published: April 2022

AbstractGraphene has inspired wide‐range research interests and practical applications due to its intriguing materials properties and versatile application prospects. Specifically, vertically oriented graphene (VG) constructed by vertically aligned nanosheets emerges as a unique material type, usually achieved through a plasma‐enhanced chemical vapor deposition (PECVD) route. The VG films possess abundant exposed active edges, large surface areas, relatively high electrical conductivity, and excellent thermal property in both in‐plane and out‐of‐plane directions. Direct synthesizing of such VG films on various functional substrates enables their transfer‐free integrations and direct applications in thermal management, sensing, energy storage and conversion, etc. In this review article, it is planned to showcase the recent advances in direct PECVD growth of VG films on some novel functional insulating substrates (e.g., glass, functional ceramics), mainly in terms of improving the electrical conductivity, enhancing the interfacial adhesion, and graphene growth orientation modulation. Meanwhile, the applications of the PECVD‐derived products in various new fields will also be discussed, such as photothermal conversion, switchable windows, light attenuation in photography, transparent heating, and thermal management for high‐power devices. Finally, current challenges and future opportunities will also be presented regarding controllable syntheses of high‐quality VG films and practical application explorations in different fields.
Reinforced Layered Double Hydroxide Oxygen‐Evolution Electrocatalysts: A Polyoxometallic Acid Wet‐Etching Approach and Synergistic Mechanism
Authors: Cai Zhengyang , Wang Ping , Zhang Jiajia , Chen Aiying , Zhang Jiangwei , Yan Ya , Wang Xianying 
Published: April 2022

AbstractNickel–iron‐based layered double hydroxides (NiFe LDHs) have attracted tremendous research and industrial interests for oxygen evolution reaction (OER) electrocatalysis. However, methodologies on simultaneous regulation of performance‐influencing factors remain scarce and their real synergistic effects are not clear enough. Herein, a versatile polyoxometallic acids (POMs) etching approach is reported to ingeniously reconstruct NiFe LDH, including 3D morphological nanotailoring, Fe3+ and α‐Ni(OH)2 active species reconfiguration, creation of multiple Ni, Fe, and O vacancies, and intercalation of POM polyanionic clusters. The experimental and theoretical data collaboratively unveil that control of the key performance‐influencing factors and their multiple synergistic mechanisms dominantly contribute to the step‐like OER performance enhancement. The reinforced electrocatalyst is further produced with low cost and high performance up to Ф180 mm in diameter, showing its feasibility and advancement of the promising configuration of NiFe LDH‐PMo12(+) II Ni@NiFe LDH(−) for alkaline anion‐exchange‐membrane electrode stack cells. Furthermore, to mathematically evaluate the evolution, a novel empirical formula is proposed for quantitative identification of structure–activity correlations, which offers an opportunity for first and fast reliability on materials screening.
Structural Reconstruction of Catalysts in Electroreduction Reaction: Identifying, Understanding, and Manipulating
Authors: Wang Wenbin , Duan Junyuan , Liu Youwen , Zhai Tianyou 
Published: April 2022

AbstractElectroreduction transformation of small molecules (CO2, N2, and H2O) into chemical feedstocks offers a promising approach to eliminate carbon emissions and harness renewable energy. Most cathodic catalysts often undergo structural transformation under operating electroreduction conditions. These structural reconstructions are reflected in changes in their catalytic activity. In‐depth understanding of the change of active sites and influence parameters of reconstruction behaviors is an essential precondition for the design of highly efficient catalysts. Despite the previous achievements, comprehensive insight toward the structural evolution mechanism in cathodic catalysts, compared to anode ones, under reaction conditions is still lacking. Herein, an overview of structural reconstruction for cathodic catalysts in terms of fundamental mechanisms, reconstruction process, advanced characterizations, and influencing parameters is provided. On this basis, the typical strategies for manipulating the structural reconfiguration of catalysts are also explicitly discussed from the catalyst structure and working environment. By delivering the mechanism, strategies, insights, and techniques, this review will provide a comprehensive understanding of the structural reconstruction of cathodic catalysts in electroreduction reactions and future guidelines for their rational development.
Boosting Electrochemical Styrene Transformation via Tandem Water Oxidation over a Single‐Atom Cr1/CoSe2 Catalyst
Authors: Dang Kun , Dong Hongliang , Wang Ligang , Jiang Mai , Jiang Sen , Sun Wenming , Wang Dingsheng , Tian Yang 
Published: April 2022

AbstractElectrocatalytic oxidation of organics using water as the oxygen source is a prospective but challenging method to produce high‐value‐added chemicals; especially, the competitive oxygen evolution reaction (OER) limits its efficiency. Herein, a tandem catalysis strategy based on a single‐atom catalyst with Cr atoms atomically dispersed at a CoSe2 support (Cr1/CoSe2) is presented. Thereinto, Co and Cr sites are endowed with a specific function to activate water and styrene respectively, and the competition between the OER and styrene oxidation is turned into mutual benefits via cooperated active sites. Under a potential of 1.6 VAg/AgCl, excellent selectivity of 95% to benzaldehyde and a high conversion rate of styrene at 88% without any exogenous oxidizing reagent are achieved. Isotopic tracing, isotope‐labeled in situ Raman spectra, and detailed theoretical calculation further reveal the tandem mechanism, showing that the transfer of *OOH intermediates from the Co to the Cr sites serves as a bridge to link the oxidation of water and styrene. This work develops a new strategy for the co‐oxidation of multi‐species based on tandem catalysis, providing novel insights for the design of single‐atom catalysts.
Universal Dynamic Liquid Interface for Healing Perovskite Solar Cells
Authors: Guo Qiyao , Duan Jialong , Zhang Junshuai , Zhang Qiaoyu , Duan Yanyan , Yang Xiya , He Benlin , Zhao Yuanyuan , Tang Qunwei 
Published: April 2022

AbstractHealing charge‐selective contact interfaces in perovskite solar cells (PSCs) highly determines the power conversion efficiency (PCE) and stability. However, the state‐of‐the‐art strategies are often static by one‐off formation of a functional interlayer, which delivers fixed interfacial properties during the subsequent operation. As a result, defects formed in‐service will gradually deteriorate the photovoltaic performances. Herein, a dynamic healing interface (DHI) is presented by incorporating a low‐melting‐point small molecule onto perovskite film surface for highly efficient and stable PSCs. Arising from the reduced non‐radiative recombination, the DHI boosts the PCE to 12.05% for an all‐inorganic CsPbIBr2 solar cell and 14.14% for a CsPbI2Br cell, as well as 23.37% for an FA0.92MA0.08PbI3 (FA = formamidinium, MA = methylammonium) cell. The solid‐to‐liquid phase conversion of DHI at elevated temperature causes a longitudinal infiltration into the bulk perovskite film to maximize the charge extraction, passivate defects at grain boundaries, and suppress ion migration. Furthermore, the stability is remarkably enhanced under air, heat, and persistent light‐irradiation conditions, paving a universal strategy for advanced perovskite‐based optoelectronics.
Monitoring Wound Healing with Topically Applied Optical NanoFlare mRNA Nanosensors
Authors: Hwang Jangsun , Seo Youngmin , Jeong Daun , Ning Xiaoyu , Wiraja Christian , Yang Lixia , Tan Chew Teng , Lee Jinhyuck , Kim Yesol , Kim Ji Won , Kim Dai Hyun , Choi Jonghoon , Lim Chin Yan , Pu Kanyi , Jang Woo Young , Xu Chenjie 
Published: April 2022

AbstractAn effective wound management strategy needs accurate assessment of wound status throughout the whole healing process. This can be achieved by examining molecular biomarkers including proteins, DNAs, and RNAs. However, existing methods for quantifying these biomarkers such as immunohistochemistry and quantitative polymerase chain reaction are usually laborious, resource‐intensive, and disruptive. This article reports the development and utilization of mRNA nanosensors (i.e., NanoFlare) that are topically applied on cutaneous wounds to reveal the healing status through targeted and semi‐quantitative examination of the mRNA biomarkers in skin cells. In 2D and 3D in vitro models, the efficacy and efficiency of these nanosensors are demonstrated in revealing the dynamic changes of mRNA biomarkers for different stages of wound development. In mouse models, this platform permits the tracking and identification of wound healing stages and a normal and diabetic wound healing process by wound healing index in real time.
DNA Walkers for Biosensing Development
Authors: Song Lu , Zhuge Ying , Zuo Xiaolei , Li Min , Wang Fang 
Published: April 2022

AbstractThe ability to design nanostructures with arbitrary shapes and controllable motions has made DNA nanomaterials used widely to construct diverse nanomachines with various structures and functions. The DNA nanostructures exhibit excellent properties, including programmability, stability, biocompatibility, and can be modified with different functional groups. Among these nanoscale architectures, DNA walker is one of the most popular nanodevices with ingenious design and flexible function. In the past several years, DNA walkers have made amazing progress ranging from structural design to biological applications including constructing biosensors for the detection of cancer‐associated biomarkers. In this review, the key driving forces of DNA walkers are first summarized. Then, the DNA walkers with different numbers of legs are introduced. Furthermore, the biosensing applications of DNA walkers including the detection‐ of nucleic acids, proteins, ions, and bacteria are summarized. Finally, the new frontiers and opportunities for developing DNA walker‐based biosensors are discussed.
Thermally Conductive AlN‐Network Shield for Separators to Achieve Dendrite‐Free Plating and Fast Li‐Ion Transport toward Durable and High‐Rate Lithium‐Metal Anodes
Authors: Guo Yue , Wu Qiang , Liu Liwei , Li Guochang , Yang Lijun , Wang Xizhang , Ma Yanwen , Hu Zheng 
Published: April 2022

AbstractLithium‐metal anodes suffer from inadequate rate and cycling performances for practical application mainly due to the harmful dendrite growth, especially at high currents. Herein a facile construction of the porous and robust network with thermally conductive AlN nanowires onto the commercial polypropylene separator by convenient vacuum filtration is reported. The so‐constructed AlN‐network shield provides a uniform thermal distribution to realize homogeneous Li deposition, super electrolyte‐philic channels to enhance Li‐ion transport, and also a physical barrier to resist dendrite piercing as the last fence. Consequently, the symmetric Li|Li cell presents an ultralong lifetime over 8000 h (20 mA cm−2, 3 mAh cm−2) and over 1000 h even at an unprecedented high rate (80 mA cm−2, 80 mAh cm−2), which is far surpassing the corresponding performances reported to date. The corresponding Li|LiFePO4 cell delivers a high specific capacity of 84.3 mAh g−1 at 10 C. This study demonstrates an efficient approach with great application potential toward durable and high‐power Li–metal batteries and even beyond.
A Comprehensive Understanding of the Aging Effects of Extreme Fast Charging on High Ni NMC Cathode
Authors: Tanim Tanvir R. , Yang Zhenzhen , Finegan Donal P. , Chinnam Parameswara R. , Lin Yulin , Weddle Peter J. , Bloom Ira , Colclasure Andrew M. , Dufek Eric J. , Wen Jianguo , Tsai Yifen , Evans Michael C. , Smith Kandler , Allen Jeffery M. , Dickerson Charles C. , Quinn Alexander H. , Dunlop Alison R. , Trask Stephen E. , Jansen Andrew N. 
Published: April 2022

AbstractAs the battery industry shifts toward high Ni content cathodes, such as LiNi0.8Mn0.1Co0.1O2 [NMC811], a complete understanding of the degradation mechanisms of NMC811 under extreme fast charging (XFC) (XFC, ≤10–15 min charging) conditions is needed. Such comprehensive understanding would identify the most critical materials gaps that need to be addressed for enabling XFC long‐life cells for electric vehicles. This study maps out the key aging mechanisms for NMC811 cycled at different XFC conditions (between 1C and 9C) for up to 1000 cycles. To acquire a fundamental understanding of utilization and degradation, cells are evaluated using a range of electrochemical techniques, and multimodal and multiscale microscopy techniques to quantify chemical, structural, and crystallographic degradation as a function of cycling conditions for the NMC cathode. When comparing NMC811 to NMC532, it is observed that NMC811 has a greater subsurface crystallographic degradation and displays a similar magnitude of subparticle cracking. However, the NMC811 maintains superior performance despite those advanced degradations. The superior cycle life performance is attributed to the NMC811 particles having radially oriented grains and improved transport properties. NMC811 shows between 4.6× and 3.15× reduction in capacity fade than NMC532 for charging rates between 4C (e.g., 15‐min charging) and 6C (10‐min charging).
A Polymerized‐Ionic‐Liquid‐Based Polymer Electrolyte with High Oxidative Stability for 4 and 5 V Class Solid‐State Lithium Metal Batteries
Authors: Fu Chengyin , Homann Gerrit , Grissa Rabeb , Rentsch Daniel , Zhao Wengao , Gouveia Tom , Falgayrat Anaïs , Lin Rongying , Fantini Sébastien , Battaglia Corsin 
Published: April 2022

AbstractPolymer solid electrolytes for solid‐state batteries typically suffer from low ionic conductivity and low oxidative stability. Herein, a polymer electrolyte based on a polymerized ionic liquid and an ionic liquid plasticizer offering simultaneously a high room‐temperature ionic conductivity of 0.8 mS cm−1 and a high oxidative stability >5.0 V versus Li+/Li, is reported. The electrolyte is compatible with lithium metal and non‐flammable upon direct flame exposure. In symmetric lithium metal cells, the electrolyte enables stable lithium plating and stripping at 0.1 mA cm−2 with a capacity of 1 mAh cm−2 per half cycle for over 1700 h at 25 °C. Cells with a lithium metal anode cycled against a state‐of‐the‐art high‐energy uncoated layered LiNi0.8Mn0.1Co0.1O2 cathode achieve an initial capacity of 162 mA h g−1 and a capacity retention of 72% after 600 cycles to an upper cut‐off voltage of 4.4 V at 25 °C. Cells with a high‐voltage spinel LiMn1.5Ni0.5O4 cathode reach an initial capacity of 132 mAh g−1 and a capacity retention of 76% after 300 cycles to an upper cut‐off voltage of 5 V at 25 °C, confirming the high oxidative stability and technological potential of this electrolyte for high‐voltage solid‐state lithium metal batteries.
Atomic‐Level Platinum Filling into Ni‐Vacancies of Dual‐Deficient NiO for Boosting Electrocatalytic Hydrogen Evolution
Authors: Yan Yaotian , Lin Jinghuang , Xu Tianxiong , Liu Baishen , Huang Keke , Qiao Liang , Liu Shude , Cao Jian , Jun Seong Chan , Yamauchi Yusuke , Qi Junlei 
Published: April 2022

AbstractDeveloping low‐cost and high‐efficiency catalysts for sustainable hydrogen production through electrocatalytic hydrogen evolution reaction (HER) is crucial yet remains challenging. Here, a strategy is proposed to fill Ni‐vacancy (Niv) sites of dual‐deficient NiO (D‐NiO‐Pt) deliberately created by Ar plasma with homogeneously distributed Pt atoms driven by oxygen vacancies (Ov). The incorporated Pt atoms filling the Niv reduce the formation energy to increase crystal stability, and subsequently combine with additional Ov to tune the electronic structure of the surrounding Ni sites. Thus, a more ideal hydrogen adsorption free energy (ΔGH*) closer to 0 of Ni sites and Pt sites can be achieved. As a result, the D‐NiO‐Pt electrode achieves superior mass activity of ≈1600 mA mg−1 (normalized by platinum) and nearly negligible loss of activity during long‐term operation, which is much better than as‐prepared Pt‐containing NiO catalysts without plasma treatment. A low overpotential of 20 mV is required for the D‐NiO‐Pt at 10 mA cm−2 in alkaline HER, outperforming that of the commercial Pt/C. In addition, the universal access to the other Ni‐based compounds including nickel phosphide (Ni2P), nickel sulfide (Ni0.96S), and nickel selenide (NiSe2) is also demonstrated by employing a vacancy‐driven Pt filling mechanism.
Indigo: A Natural Molecular Passivator for Efficient Perovskite Solar Cells
Authors: Guo Junjun , Sun Jianguo , Hu Long , Fang Shiwen , Ling Xufeng , Zhang Xuliang , Wang Yao , Huang Hehe , Han Chenxu , Cazorla Claudio , Yang Yingguo , Chu Dewei , Wu Tom , Yuan Jianyu , Ma Wanli 
Published: April 2022

AbstractOrganic–inorganic hybrid lead halide perovskite solar cells have made unprecedented progress in improving photovoltaic efficiency during the past decade, while still facing critical stability challenges. Herein, the natural organic dye Indigo is explored for the first time to be an efficient molecular passivator that assists in the preparation of high‐quality hybrid perovskite film with reduced defects and enhanced stability. The Indigo molecule with both carbonyl and amino groups can provide bifunctional chemical passivation for defects. In‐depth theoretical and experimental studies show that the Indigo molecules firmly binds to the perovskite surfaces, enhancing the crystallization of perovskite films with improved morphology. Consequently, the Indigo‐passivated perovskite film exhibits increased grain size with better uniformity, reduced grain boundaries, lowered defect density, and retarded ion migration, boosting the device efficiency up to 23.22%, and ≈21% for large‐area device (1 cm2). Furthermore, the Indigo passivation can enhance device stability in terms of both humidity and thermal stress. These results provide not only new insights into the multipassivation role of natural organic dyes but also a simple and low‐cost strategy to prepare high‐quality hybrid perovskite films for optoelectronic applications based on Indigo derivatives.
Simultaneous Incorporation of V and Mn Element into Polyanionic NASICON for High Energy‐Density and Long‐Lifespan Zn‐Ion Storage
Authors: Wu Zeyi , Ye Fei , Liu Qiang , Pang Ruilvjing , Liu Yang , Jiang Le , Tang Zilong , Hu Linfeng 
Published: April 2022

AbstractAqueous Zn‐ion battery (AZIB) has attracted huge attention due to its distinct advantages such as abundant zinc sources, low development cost, high security, and environmental friendliness compared to traditional commercialized batteries. Developing novel cathode materials with high energy density and long lifespan is very important for the practical application of AZIB in the coming years. Herein, V and Mn elements are simultaneously incorporated into the NASICON host to make use of the electrochemical redox reaction in both V and Mn transition metal elements for aqueous Zn‐ion storage. A significant increase in both capacity and working voltage has been observed after Mn doping into Na3V2(PO4)3 to form Na4VMn(PO4)3. Taking advantage of the merits of both high capacity and high voltage, the Na4VMn(PO4)3@Graphene cathode delivers an optimal energy density of 309.7 Wh kg−1 with very stable cycle performance (89.1% capacity retention after 3000 cycles at 5.0 A g−1). A two‐step electron transfer mechanism between V4+/V3+ and Mn3+/Mn2+ redox couple in Na4VMn(PO4)3 has been revealed during the electrochemical process for Zn‐ion storage.