bluuebunny/crossref_metadata_2025_split huggingface dataset:
Boosting O2 Reduction and H2O Dehydrogenation Kinetics: Surface N‐Hydroxymethylation of g‐C3N4 Photocatalysts for the Efficient Production of H2O2
Authors: Liu Binyao , Du Jinyan , Ke Gaili , Jia Bi , Huang Yujie , He Huichao , Zhou Yong , Zou Zhigang 
Published: December 2021

Abstractg‐C3N4 photocatalysis is a safe and green approach for H2O2 production, but the activity of pristine g‐C3N4 photocatalysts is unsatisfactory. At present, most of the modifications on g‐C3N4 photocatalysts for H2O2 production have focused on thermodynamic processes, few have considered the kinetic aspects. Herein, the surface N‐hydroxymethylation of g‐C3N4 photocatalysts for the efficient kinetic production of H2O2 is reported. Through the reaction of formaldehyde with the amino moieties (–NH2) on the g‐C3N4 surface, N‐hydroxymethyls groups (‐NH‐CH2‐OH) are introduced on typical g‐C3N4 photocatalysts. Relative to the pristine g‐C3N4 photocatalysts, the modified g‐C3N4 photocatalysts have over 1280% higher activity for H2O2 production in pure water system, and impressive solar‐to‐chemical conversion efficiency. The experimental investigations and theoretical calculations reveal that the introduction of ‐NH‐CH2‐OH on the g‐C3N4 photocatalysts does not change their morphology, light absorption intensity and edges, band positions, charge separation and transfer properties, but markedly improved the H2O dehydrogenation and O2 adsorption properties of g‐C3N4. As a result, the reduction kinetics of O2 to H2O2 on the g‐C3N4 photocatalysts with ‐NH‐CH2‐OH is more energetically favorable. This work provides a useful reference and inspiration to achieve the effective modification of g‐C3N4 or other metal‐free photocatalysts from the kinetic perspective.
Ultrarapid Method for Coating Electrochemical Sensors with Antifouling Conductive Nanomaterials Enables Highly Sensitive Multiplexed Detection in Whole Blood
Authors: Timilsina Sanjay S. , Durr Nolan , Yafia Mohamed , Sallum Hani , Jolly Pawan , Ingber Donald E. 
Published: December 2021

AbstractThe commercialization of electrochemical (EC)‐sensors for medical diagnostics is currently limited by their rapid fouling in biological fluids, and use of potential antifouling coatings is hindered by the complexity and cost of application methods. Here, a simple ultrafast (< 1 min) method is described for coating EC‐sensors with cross‐linked bovine serum albumin infused with conductive, pentaamine‐functionalized, graphene particles that can be stored at room temperature for at least 20‐weeks, which provides unprecedented sensitivity and selectivity for diagnostic applications. The antifouling coating is applied directly on‐chip using rapid heating via simple dip‐coating, which provides unprecedented high levels of electrode conductivity for up to 9‐weeks in unprocessed biological samples. This method is leveraged to develop a multiplexed platform for detecting clinically relevant biomarkers including myocardial infarction and traumatic brain injury using only 15 µL of blood. Single‐digit pg mL−1 sensitivity is obtained within minutes in unprocessed human plasma and whole blood, which is faster and at least 50 times more sensitive than traditional enzyme‐linked immunosorbent assays, and the signal generated is stable enough to be measured after 1 week of storage. The multiplexed EC‐sensor platform is validated by analyzing 22 patient samples and demonstrating excellent correlation with reported clinical values.
Sunlight‐Coordinated High‐Performance Moisture Power in Natural Conditions
Authors: Bai Jiaxin , Huang Yaxin , Wang Haiyan , Guang Tianlei , Liao Qihua , Cheng Huhu , Deng Shanhao , Li Qikai , Shuai Zhigang , Qu Liangti 
Published: December 2021

AbstractIt is a challenge to spontaneously harvest multiple clean sources from the environment for upgraded energy‐converting systems. The ubiquitous moisture and sunlight in nature are attractive for sustainable power generation especially. A high‐performance light‐coordinated “moist‐electric generator” (LMEG) based on the rational combination of a polyelectrolyte and a phytochrome is herein developed. By spontaneous adsorption of gaseous water molecules and simultaneous exposure to sunlight, a piece of 1 cm2 composite film offers an open‐circuit voltage of 0.92 V and a considerable short‐circuit current density of up to 1.55 mA cm−2. This record‐high current density is about two orders of magnitude improvement over that of most conventional moisture‐enabled systems, which is caused by moisture‐induced charge separation accompanied with photoexcited carrier migration, as confirmed by a dynamic Monte Carlo device simulation. Flexible devices with customizable size are available for large‐scale integration to effectively work under a wide range of relative humidity (about 20–100%), temperature (10–80 °C), and light intensity (30–200 mW cm−2). The wearable and portable LMEGs provide ample power supply in natural conditions for indoor and outdoor electricity‐consuming systems. This work opens a novel avenue to develop sustainable power generation through collecting multiple types of natural energy by a single hybrid harvester.
Ionic Liquid Treatment for Highest‐Efficiency Ambient Printed Stable All‐Inorganic CsPbI3 Perovskite Solar Cells
Authors: Du Yachao , Tian Qingwen , Chang Xiaoming , Fang Junjie , Gu Xiaojing , He Xilai , Ren Xiaodong , Zhao Kui , Liu Shengzhong (Frank) 
Published: December 2021

AbstractAll‐inorganic cesium lead triiodide (CsPbI3) perovskite is well known for its unparalleled stability at high temperatures up to 500 °C and under oxidative chemical stresses. However, upscaling solar cells via ambient printing suffers from imperfect crystal quality and defects caused by uncontrollable crystallization. Here, the incorporation of a low concentration of novel ionic liquid is reported as being promising for managing defects in CsPbI3 films, interfacial energy alignment, and device stability of solar cells fabricated via ambient blade‐coating. Both theoretical simulations and experimental measurements reveal that the ionic liquid successfully regulates the perovskite thin‐film growth to decrease perovskite grain boundaries, strongly coordinates with the undercoordinated Pb2+ to passivate iodide vacancy defects, aligns the interface to decrease the energy barrier at the electron‐transporting layer, and relaxes the lattice strain to promote phase stability. Consequently, ambient printed CsPbI3 solar cells with power conversion efficiency as high as 20.01% under 1 sun illumination (100 mW cm−2) and 37.24% under indoor light illumination (1000 lux, 365 µW cm−2) are achieved; both are the highest for printed all‐inorganic cells for corresponding applications. Furthermore, the bare cells show an impressive long‐term ambient stability with only ≈5% PCE degradation after 1000 h aging under ambient conditions.
A Stiffness‐Switchable, Biomimetic Smart Material Enabled by Supramolecular Reconfiguration
Authors: Zhao Dawei , Pang Bo , Zhu Ying , Cheng Wanke , Cao Kaiyue , Ye Dongdong , Si Chuanling , Xu Guangwen , Chen Chaoji , Yu Haipeng 
Published: December 2021

AbstractIn nature, stiffness‐changing behavior is essential for living organisms, which, however, is challenging to achieve in synthetic materials. Here, a stiffness‐changing smart material, through developing interchangeable supramolecular configurations inspired from the dermis of the sea cucumber, which shows extreme, switchable mechanical properties, is reported. In the hydrated state, the material, possessing a stretched, double‐stranded supramolecular network, showcases a soft‐gel behavior with a low stiffness and high pliability. Upon the stimulation of ethanol to transform into the coiled supramolecular configuration, it self‐adjusts to a hard state with nearly 500‐times enhanced stiffness from 0.51 to 243.6 MPa, outstanding load‐bearing capability (over 35 000 times its own weight), and excellent puncture/impact resistance with a specific impact strength of ≈116 kJ m−2 (g cm−3)−1 (higher than some metals and alloys such as aluminum, and even comparable to the commercially available protective materials such as D3O and Kevlar). Moreover, this material demonstrates reconfiguration‐dependent self‐healing behavior and designable formability, holding great promise in advanced engineering fields that require both high‐strength durability and good formability. This work may open up a new perspective for the development of self‐regulating materials from supramolecular‐scale configuration regulation.
Reshaping the Tumor Immune Microenvironment Based on a Light‐Activated Nanoplatform for Efficient Cancer Therapy
Authors: Yang Zebin , Luo Yu , Yu Huizhu , Liang Kaicheng , Wang Miao , Wang Qigang , Yin Bo , Chen Hangrong 
Published: December 2021

AbstractThe immunosuppressive tumor microenvironment (TME) always causes poor antitumor immune efficacy, prone to relapse and metastasis. Herein, novel poly(vinylpyrrolidone) (PVP) modified BiFeO3/Bi2WO6 (BFO/BWO) with a p–n type heterojunction is constructed for reshaping the immunosuppressive TME. Reactive oxygen species can be generated under light activation by the well‐separated hole (h+)–electron (e−) pairs owing to the heterojunction in BFO/BWO‐PVP NPs. Interestingly, h+ can trigger the decomposition of H2O2 to generate O2 for alleviating tumor hypoxia, which not only sensitizes photodynamic therapy (PDT) and radiotherapy (RT), but also promotes tumor‐associated macrophages (TAMs) polarization from M2 to M1 phenotype, which is beneficial to decrease the expression of HIF‐1α. Importantly, such a light‐activated nanoplatform, combining with RT can efficiently activate and recruit cytotoxic T lymphocytes to infiltrate in tumor tissues, as well as stimulate TAMs to M1 phenotype, dramatically reverse the immunosuppressive TME into an immunoactive one, and further boost immune memory responses. Moreover, BFO/BWO‐PVP NPs also present high performance for computed tomography imaging contrast. Taken together, this work offers a novel paradigm for achieving O2 self‐supply of inorganic nanoagents and reshaping of the tumor immune microenvironment for effective inhibition of cancer as well as metastasis and recurrence.
Monolithic All‐Perovskite Tandem Solar Cells with Minimized Optical and Energetic Losses
Authors: Datta Kunal , Wang Junke , Zhang Dong , Zardetto Valerio , Remmerswaal Willemijn H. M. , Weijtens Christ H. L. , Wienk Martijn M. , Janssen René A. J. 
Published: December 2021

AbstractPerovskite‐based multijunction solar cells are a potentially cost‐effective technology that can help surpass the efficiency limits of single‐junction devices. However, both mixed‐halide wide‐bandgap perovskites and lead‐tin narrow‐bandgap perovskites suffer from non‐radiative recombination due to the formation of bulk traps and interfacial recombination centers which limit the open‐circuit voltage of sub‐cells and consequently of the integrated tandem. Additionally, the complex optical stack in a multijunction solar cell can lead to losses stemming from parasitic absorption and reflection of incident light which aggravates the current mismatch between sub‐cells, thereby limiting the short‐circuit current density of the tandem. Here, an integrated all‐perovskite tandem solar cell is presented that uses surface passivation strategies to reduce non‐radiative recombination at the perovskite‐fullerene interfaces, yielding a high open‐circuit voltage. By using optically benign transparent electrode and charge‐transport layers, absorption in the narrow‐bandgap sub‐cell is improved, leading to an improvement in current‐matching between sub‐cells. Collectively, these strategies allow the development of a monolithic tandem solar cell exhibiting a power‐conversion efficiency of over 23%.
Physical Implementation of Reservoir Computing through Electrochemical Reaction
Authors: Kan Shaohua , Nakajima Kohei , Asai Tetsuya , Akai‐Kasaya Megumi 
Published: December 2021

AbstractNonlinear dynamical systems serving reservoir computing enrich the physical implementation of computing systems. A method for building physical reservoirs from electrochemical reactions is provided, and the potential of chemical dynamics as computing resources is shown. The essence of signal processing in such systems includes various degrees of ionic currents which pass through the solution as well as the electrochemical current detected based on a multiway data acquisition system to achieve switchable and parallel testing. The results show that they have respective advantages in periodic signals and temporal dynamic signals. Polyoxometalate molecule in the solution increases the diversity of the response current and thus improves their abilities to predict periodic signals. Conversely, distilled water exhibits great computing power in solving a second‐order nonlinear problem. It is expected that these results will lead to further exploration of ionic conductance as a nonlinear dynamical system and provide more support for novel devices as computing resources.
Thickness and Morphology Dependent Electrical Properties of ALD‐Synthesized MoS2FETs
Authors: Mahlouji Reyhaneh , Verheijen Marcel A. , Zhang Yue , Hofmann Jan P. , Kessels Wilhelmus. M. M.(Erwin) , Bol Ageeth A. 
Published: December 2021

AbstractMoS2is a layered 2D semiconductor with thickness‐dependent electrical properties. Often, 6–12 nm of MoS2are advised to be used as the channel material in field‐effect transistors (FETs) for achieving an optimal device electrical performance. However, this notion is based on exfoliated MoS2flakes that cannot be employed for large‐area and wafer‐scale applications. In this work, the thickness‐dependent electrical properties of atomic layer deposition (ALD)‐based MoS2FETs are studied. A two‐step approach is used for the synthesis of MoS2, wherein large‐area and thickness‐controlled MoOxfilms are initially grown using plasma‐enhanced (PE‐)ALD and subsequently sulfurized in H2S gas. The number of MoOxPE‐ALD cycles is varied systematically to obtain MoS2films with a thickness range of 1–10 nm. Current–voltage (I–V) characterization of the fabricated MoS2FETs with various channel thicknesses reveals that ≈1.2 nm MoS2suffices in attaining the best device electrical performance. Scanning transmission electron microscopy imaging elucidates that the synthetic MoS2films are polycrystalline and the resultant ≈1.2 nm of MoS2are not completely continuous. The empty areas in the polycrystalline MoS2network can serve as locations for side contact formation, leading to substantial improvements in the device metrics fabricated from such ultrathin MoS2films.
Hybrid Design of Bulk‐Na Metal Anode to Minimize Cycle‐Induced Interface Deterioration of Solid Na Metal Battery
Authors: Cao Keshuang , Zhao Xitong , Chen Jian , Xu Ben Bin , Shahzad Muhammad Wakil , Sun Wenping , Pan Hongge , Yan Mi , Jiang Yinzhu 
Published: December 2021

AbstractThe pursuit for high‐energy and intrinsically safe energy storage is significantly driving the development of solid‐state alkali metal batteries. The interfacial contact between the metal anode and the solid electrolyte plays a key role in enabling stable cycling of solid batteries. However, the sluggish alkali atom replenishment rate during stripping unavoidably leads to the interface deterioration that destroys the initial physical contact by forming interfacial voids and triggering the dendrite growth. Herein, a hybrid bulk Na anode approach is proposed by incorporating an ion‐conducting phase into a metallic Na matrix, constructing an abundant interfacial electrochemical reaction area and enabling a balanced Na replenishment and consumption to minimize cycle‐induced interface deterioration. Specific attention is paid to the effects of the second phase on the wettability and creep ability of hybrid Na metal. A high critical current density (3.1 mA cm‐2) and long cycling life (6000 h in 0.5 mA cm‐2) are achieved for the symmetric cells. Full cells coupling the hybrid anode with the Na3V2(PO4)3/C cathode deliver excellent cyclability over 7300 cycles at a high rate of 5 C. The viewpoint of balancing the consumption and replenishment rate of metal atoms paves a new way for designing cycle‐stable anode/electrolyte interface in solid‐state batteries.
Recent Progress of Critical Interface Engineering for Highly Efficient and Stable Perovskite Solar Cells
Authors: Li Yahong , Xie Haibing , Lim Eng Liang , Hagfeldt Anders , Bi Dongqin 
Published: December 2021

AbstractOrganic–inorganic lead halide perovskite solar cells (PSCs) have demonstrated enormous potential as a new generation of solar‐based renewable energy. Although their power conversion efficiency (PCE) has been boosted to a spectacular record value, the long‐term stability of efficient PSCs is still the dominating concern that hinders their commercialization. Notably, interface engineering has been identified as a valid strategy with extraordinary achievements for enhancing both efficiency and stability of PSCs. Herein, the latest research advances of interface engineering for various interfaces are summarized, and the basic theory and multifaceted roles of interface engineering for optimizing device properties are analyzed. As a highlight, the authors provide their insights on the deposition strategy of interlayers, application of first‐principle calculation, and challenges and solutions of interface engineering for PSCs with high efficiency and stability toward future commercialization.
Sulfurized Carbon Composite with Unprecedentedly High Tap Density for Sodium Storage
Authors: Jo Chang‐Heum , Yu Jun Ho , Kim Hee Jae , Hwang Jang‐Yeon , Kim Ji‐Young , Jung Hun‐Gi , Myung Seung‐Taek 
Published: December 2021

AbstractA novel sulfurized carbon decorated by terephthalic acid (TPA) and polyacrylonitrile (PAN), with unprecedently high tap density (≈1.02 g cm−3), is investigated. Room‐temperature sodium–sulfur batteries offer high energy density; however, the dissolution of the polysulfide is a major factor hindering their commercialization. This dissolution problem can be tolerated by inhibiting the formation of polysulfide through binding sulfur to the carbon structure of PAN. Low sulfur content and low volumetric energy density in the composite are other drawbacks to be resolved. Heat‐treated TPA induces a high‐density carbonaceous material with high conductivity. This TPA is partly replaced by PAN, and the produced carbon and sulfur are composited with dehydrated polyacrylonitrile (CS–DPAN), which exhibits higher conductivity and surface area than the sulfurized dehydrated polyacrylonitrile (S–DPAN). The CS–DPAN composite electrode exhibits excellent electrochemical performance, and the resulting volumetric capacity is also superior to that of the S–DPAN material electrode. Operando Raman and operando X‐ray diffraction analyses confirm that the increased capacity is realized via the avoidance of parasitic C60Na3 formation formed below 1 V, by adjusting the operation voltage range. This finding demonstrates the feasibility of carbon–sulfur composites as a high‐energy electrode material for rechargeable sodium batteries.
A High‐Performance Dual‐Ion Battery‐Supercapacitor Hybrid Device Based on LiCl in Ion Liquid Dual‐Salt Electrolyte
Authors: Xiong Zhangyi , Guo Peijing , Yang Yushan , Yuan Shaoyu , Shang Ningzhao , Wang Chun , Zhang Yufan , Wang Huan , Gao Yongjun 
Published: December 2021

AbstractA dual‐ion battery‐supercapacitor hybrid device (DIB‐SCHD), cleverly integrating a dual‐ion battery (DIB) and a supercapacitor (SC), is expected to endow both the high energy density of dual‐ion battery and the high power density of supercapacitor. Benefitting from the similar features of the electrolyte and symmetrical electrode configuration, a state‐of‐the‐art DIB‐SCHD is developed by using N‐doped micropores‐dominant carbon(N‐MPC) as the electrode and LiCl in a room‐temperature ion liquid hybrid as the electrolyte, which deliver an ultrahigh mass capacitance of 374 F g−1 with a high voltage of 3.5 V and a remarkable specific energy of 208 Wh kg−1 at 1144 W kg−1 and an ultrahigh specific power of 22834 W kg−1 at 77 Wh kg−1. Combined with ex situ characterizations and theoretical calculations, the assembled DIB‐SCHD presents a synergistic energy storage mechanism simultaneously involving ion intercalation/deintercalation and adsorption/desorption processes, which can promote the reaction kinetics and achieve exceptional electrochemical performance. The perfect integration of the dual‐ion battery‐type and supercapacitor‐type electrodes provides a new strategy toward high energy and power density electrochemical energy storage devices.
Ionic‐Liquid‐Perovskite Capping Layer for Stable 24.33%‐Efficient Solar Cell
Authors: Zhu Xuejie , Yang Shaoan , Cao Yuexian , Duan Lianjie , Du Minyong , Feng Jiangshan , Jiao Yuxiao , Jiang Xiao , Sun Youming , Wang Hui , Zuo Shengnan , Liu Yucheng , Liu Shengzhong (Frank) 
Published: December 2021

AbstractMetal‐halide perovskite has emerged as an effective photovoltaic material for its high power conversion efficiency (PCE), low cost and straightforward fabrication techniques. Unfortunately, its long‐term operational durability, mainly affected by halide ion migration and undercoordinated Pb2+ is still the bottleneck for its large‐scale commercialization. In this work, an ionic liquid (IL) is designed to effectively cap the grain surface for improved stability and reduced trap density. More specifically, the Br− in the IL passivates the undercoordinated Pb2+ by chemically bonding to it, resulting in a thin layer of ionic‐liquid‐perovskite formed on the surface, leading to improved photovoltaic performance and better stability. Specifically, the solar cell exhibits an open‐circuit voltage of 1.192 V and PCE of 24.33% under one‐sun illumination with negligible hysteresis, and a large area (10.75 cm2) integrated module achieves PCE of 20.33%. Moreover, the bare device maintains over 90% of its initial efficiency after 700 h of aging at 65 °C. It also shows outstanding stability with only about 10% degradation after being exposed to the ambient environment for 1000 h. The superior efficiency and stability demonstrate that the present IL passivating strategy is a promising approach for high‐performance large area perovskite solar cell applications.