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| Open AccessIn situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction
The electrochemical oxygen reduction reaction plays an important role in new energy technologies such as fuel cells and metal-air batteries. Here the authors present a cobalt catalyst with a symmetry-broken Cl−Co−N4 moiety capable of dynamically modulating electron occupancy at active sites during practical reaction conditions to optimize oxygen reduction performance.
- Meihuan Liu
- , Jing Zhang
- & Qinghua Liu
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Article
| Open AccessStable water splitting using photoelectrodes with a cryogelated overlayer
Photoelectrodes made of earth-abundant materials can contribute to low-cost and carbon-free hydrogen production, but suffer from a short lifetime. Here the authors report cryogel overlayer to increase the operation time of the device by regulating evolving hydrogen bubble dynamics.
- Byungjun Kang
- , Jeiwan Tan
- & Hyungsuk Lee
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Article
| Open AccessLiquid Madelung energy accounts for the huge potential shift in electrochemical systems
Electrode potential in any electrochemical systems has long been discussed by classical Debye-Hückel theory which holds only under extremely dilute concentrations. Here, the authors establish the concept ‘liquid Madelung potential’ to comprehensively describe the potential shift at practical concentrations.
- Norio Takenaka
- , Seongjae Ko
- & Atsuo Yamada
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Article
| Open AccessKirkendall effect-induced uniform stress distribution stabilizes nickel-rich layered oxide cathodes
Nickel-rich layered oxide cathodes offer high energy density yet suffer from mechanical degradation during (de)lithiation. Here, the authors present a strategy that leverages the Kirkendall effect to equalize stress within the cathode particles, thereby stabilizing their structure and enhancing the cycling stability.
- Ziyao Gao
- , Chenglong Zhao
- & Baohua Li
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Article
| Open AccessCALPHAD accelerated design of advanced full-Zintl thermoelectric device
Based on the CALPHAD method, authors propose an effective screening strategy for thermoelectric contact materials, realizing a high efficiency of ~11% (at ∆T = 430 K) for the full-Zintl phase thermoelectric device.
- Li Yin
- , Xiaofang Li
- & Qian Zhang
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Article
| Open AccessPromoting high-voltage stability through local lattice distortion of halide solid electrolytes
Solid electrolytes play a crucial role as ion conductors and separator between electrodes in all-solid-state batteries. Here, the authors report a high-entropy halide solid electrolyte, which reveals the structure evolution with the increasing configurational entropy and improves the high-voltage stability.
- Zhenyou Song
- , Tengrui Wang
- & Wei Luo
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Article
| Open AccessOxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy
Direct use of flue gas for the electrocatalytic CO2 reduction reaction is desirable but severely limited by the thermodynamically favorable oxygen reduction reaction. Here the authors report an oxygen passivation strategy to improve electrocatalytic CO2 reduction reaction under aerobic conditions using a covalent organic frameworks with a photoswitching unit.
- Hong-Jing Zhu
- , Duan-Hui Si
- & Yuan-Biao Huang
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Article
| Open AccessIntegrating hydrogen utilization in CO2 electrolysis with reduced energy loss
Electrochemical CO2 reduction is a promising method of producing sustainable chemicals and fuels, yet is highly energy intensive. Here, the authors couple CO2 electrolysis with hydrogen oxidation using a Ni(OH)2/NiOOH auxiliary electrode to enhance energy efficiency.
- Xiaoyi Jiang
- , Le Ke
- & Ning Yan
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Article
| Open AccessCa-dimers, solvent layering, and dominant electrochemically active species in Ca(BH4)2 in THF
Alternatives to lithium-ion electrochemistry present challenges due to undesirable phenomena at the electrode-electrolyte interface. Through simulations, the authors find that the performance of a calcium-based electrolyte is driven entirely by molecular-scale processes within approximately 1 nm of the electrode.
- Ana Sanz Matias
- , Fabrice Roncoroni
- & David Prendergast
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Article
| Open AccessIodide manipulation using zinc additives for efficient perovskite solar minimodules
Interstitial iodides are the most critical type of defects in perovskite solar cells that limits efficiency and stability. Here, the authors introduce small amount of zinc trifluoromethane sulfonate to control iodide defects, facilitating fabrication of minimodules with efficiencies of over 19%.
- Md Aslam Uddin
- , Prem Jyoti Singh Rana
- & Jinsong Huang
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Article
| Open AccessHierarchical Li electrochemistry using alloy-type anode for high-energy-density Li metal batteries
Utilizing an ultra-thin Li anode with a thickness below 50 μm is crucial for enhancing the energy density of batteries. Here, the authors develop a finely tunable, thin alloy-based Li anode that features a hierarchical Li electrochemistry, enabling stable cycling and superior energy density in Li metal batteries.
- Jiaqi Cao
- , Yuansheng Shi
- & Xia Lu
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Article
| Open AccessMicroenvironment reconstitution of highly active Ni single atoms on oxygen-incorporated Mo2C for water splitting
The comprehensive understanding of complex catalytic mechanisms under harsh reaction conditions for efficient bifunctional single-atom electrocatalysts remain challenging. Here the authors found microenvironment reconsitution of highly active Ni single atoms on oxygen-incorporated Mo2C for water splitting.
- Mengyun Hou
- , Lirong Zheng
- & Chen Chen
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Article
| Open AccessStructurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes
O2-type Li-rich layered cathodes suppress voltage decay and aid in oxygen redox research. Here, the authors report trilateral relationship among anionic redox utilization, bulk chemo-mechanical degradation, and electrochemical fading, which can be mitigated by balancing the redox center capabilities.
- Ho-Young Jang
- , Donggun Eum
- & Kisuk Kang
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Article
| Open AccessReal-time monitoring polymerization degree of organic photovoltaic materials toward no batch-to-batch variations in device performance
Polymerization degree plays a vital role in controlling material properties and batch-to-batch variations in device performance of polymer solar cells. Here, authors develop in-situ photoluminescence system in tandem to track and estimate the polymerization degree of organic photovoltaic materials.
- Lin-Yong Xu
- , Wei Wang
- & Jie Min
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Article
| Open AccessTailoring tokamak error fields to control plasma instabilities and transport
Error fields in tokamak appear due to the imperfections and misalignment of the coils generating magnetic field. Here the authors demonstrate use of error field correction to control the plasma transport and instabilities in a tokamak - KSTAR.
- SeongMoo Yang
- , Jong-Kyu Park
- & Won-Ha Ko
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Article
| Open AccessSolvation-property relationship of lithium-sulphur battery electrolytes
In the Li-S battery, a promising next-generation battery chemistry, electrolytes are vital because of solvated polysulfide species. Here, the authors investigate solvation-property relationships via the measurement of solvation free energy of the electrolytes, guiding advanced electrolyte design for Li-S batteries.
- Sang Cheol Kim
- , Xin Gao
- & Yi Cui
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Article
| Open AccessLarge-area, untethered, metamorphic, and omnidirectionally stretchable multiplexing self-powered triboelectric skins
Stretchable sensor networks with multiplexing designs can result in misrecognition due to electrical signal interferences from the sensing nodes and internal circuits. Here, Shao et al. show an untethered triboelectric electronic skin with an elastic composite-based shield layer for lower misrecognition rate.
- Beibei Shao
- , Ming-Han Lu
- & Ying-Chih Lai
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Article
| Open AccessHigh-performance cryo-temperature ionic thermoelectric liquid cell developed through a eutectic solvent strategy
The authors make an ionic thermoelectric cell with a eutectic solvent of formamide that can operate at temperatures as low as −35 °C by applying hydrophilic and gold coated treatments to the electrode and introducing a thermal separator.
- Shuaihua Wang
- , Yuchen Li
- & Weishu Liu
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Article
| Open AccessNeural network enabled nanoplasmonic hydrogen sensors with 100 ppm limit of detection in humid air
Detecting hydrogen gas in humid air is an unresolved challenge of significant importance for the safe implementation of hydrogen (energy) technologies. Here, authors demonstrate how the use of neural networks enables the sensing of hydrogen in highly humid air with a detection limit of 100 ppm.
- David Tomeček
- , Henrik Klein Moberg
- & Christoph Langhammer
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Article
| Open AccessHigh voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes
Micro-sized silicon are promising anode materials due to low-cost and high-energy, yet their application is hindered by inaccessible electrolytes. Here, the authors report sulfolane-based electrolytes that form silicon-phobic interphases and enable high-voltage pouch cells to achieve superior cycle life.
- Ai-Min Li
- , Zeyi Wang
- & Chunsheng Wang
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Article
| Open AccessThe role of interfacial donor–acceptor percolation in efficient and stable all-polymer solar cells
The underlying charge generation dynamics and structure-property relationships in organic solar cells are not fully understood. Here, the authors demonstrate that interfacial donor-acceptor percolation plays a key role in enabling both high charge generation efficiency and device stability.
- Zhen Wang
- , Yu Guo
- & Philip C. Y. Chow
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Article
| Open AccessRedox-tunable isoindigos for electrochemically mediated carbon capture
Electrochemically-mediated carbon capture has good energy efficiency and potential in carbon dioxide separation, but optimisation of these systems is challenging. Here, the authors report the use of isoindigo derivatives to give fine-tuned interactions with CO2 for carbon capture methods.
- Xing Li
- , Xunhua Zhao
- & Yayuan Liu
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Article
| Open AccessCapacitive tendency concept alongside supervised machine-learning toward classifying electrochemical behavior of battery and pseudocapacitor materials
Analysis of capacitive behavior of electrode materials used in batteries and pseudocapacitors is challenging. Here, authors report an electrochemical signal analysis method available as an online tool to classify the charge storage behavior of a material as battery-like or a pseudocapacitor-like.
- Siraprapha Deebansok
- , Jie Deng
- & Olivier Fontaine
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Article
| Open AccessImplanting oxophilic metal in PtRu nanowires for hydrogen oxidation catalysis
Designing an efficient electrocatalyst of hydrogen oxidation reaction is highly critical for anion exchange membrane fuel cells. Here the authors report implanting oxophilic metal atoms in PtRu nanowires to significantly improve the mass activity, stability, and resistance to CO-poisoning for hydrogen oxidation.
- Zhongliang Huang
- , Shengnan Hu
- & Xiaoqing Huang
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Article
| Open AccessPotential and electric double-layer effect in electrocatalytic urea synthesis
Electrochemical urea synthesis presents a promising alternative to conventional synthesis methods, yet the elusive mechanism hindered its development. Here, the authors take copper as an example to explore the potential and electric double-layer effect in electrocatalytic urea synthesis, and reveal two essential strategies to promote the efficiency of urea synthesis.
- Qian Wu
- , Chencheng Dai
- & Zhichuan J. Xu
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Article
| Open AccessDesigning lithium halide solid electrolytes
The pursuit of all-solid-state batteries has motivated advancements in materials design. Here, the authors present a methodology demonstrating that ionic potential effectively captures crucial interactions within halide materials, guiding the design of the new materials with enhanced performance.
- Qidi Wang
- , Yunan Zhou
- & Marnix Wagemaker
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Article
| Open AccessSubtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material
Direct recycling or upcycling is promising for sustainable battery resource management. Here, the authors report a subtractive transformation strategy for upcycling spent cathode materials to high-performance 5 V-class cathodes, reducing reliance on rare elements for the sustainable Li-ion battery industry.
- Jun Ma
- , Junxiong Wang
- & Guangmin Zhou
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Article
| Open AccessSelf-assembled hydrated copper coordination compounds as ionic conductors for room temperature solid-state batteries
The design of inorganic-organic hybrid solid-state electrolytes is expected to merge the merits of both inorganic and organic material. Here, the authors craft Li-ion-implanted copper maleate hydrate nanoflakes via a bottom-up self-assembly approach to reveal superior room-temperature Li-ion conductivity.
- Xiao Zhan
- , Miao Li
- & Li Zhang
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Article
| Open AccessAvoiding ecosystem and social impacts of hydropower, wind, and solar in Southern Africa’s low-carbon electricity system
Avoiding the most damaging land use and freshwater impacts of solar PV, wind, and hydropower development while halving carbon emissions by 2040 in the Southern Africa region is not only possible but incurs only modest (3-6%) system cost increases.
- Grace C. Wu
- , Ranjit Deshmukh
- & Kudakwashe Ndhlukula
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Article
| Open AccessOptimizing potassium polysulfides for high performance potassium-sulfur batteries
Potassium-sulfur battery are promising materials for next-generation high energy, low cost batteries. Here the authors explore a tungsten based catalytic composite for optimizing potassium polysulfides and improve K-S electrochemistry in batteries
- Wanqing Song
- , Xinyi Yang
- & Wenbin Hu
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Comment
| Open AccessThe rise of high-entropy battery materials
The emergence of high-entropy materials has inspired the exploration of novel materials in diverse technologies. In electrochemical energy storage, high-entropy design has shown advantageous impacts on battery materials such as suppressing undesired short-range order, frustrating energy landscape, decreasing volumetric change and reducing the reliance on critical metals. This comment addresses the definition and potential improper use of the term “high entropy” in the context of battery materials design, highlights the unique properties of high-entropy materials in battery applications, and outlines the remaining challenges in the synthesis, characterization, and computational modeling of high-entropy battery materials.
- Bin Ouyang
- & Yan Zeng
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Article
| Open AccessWaterproof and ultraflexible organic photovoltaics with improved interface adhesion
Waterproof flexible organic solar cells without compromising mechanical flexibility and conformability remains challenging. Here, the authors demonstrate in-situ growth of hole-transporting layer to strengthen interfacial and thermodynamic adhesion for better waterproofness in 3 μm-thick devices.
- Sixing Xiong
- , Kenjiro Fukuda
- & Takao Someya
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Article
| Open AccessIntegrated energy storage and CO2 conversion using an aqueous battery with tamed asymmetric reactions
A system integrating CO2 conversion and energy storage holds great promise, but faces a major challenge due to degraded catalysts on charge. Here, the authors present a highly efficient energy storage and CO2 reduction method in an aqueous battery, achieved through oxidation of reducing molecules.
- Yumei Liu
- , Yun An
- & Quanquan Pang
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Article
| Open AccessImpact of palladium/palladium hydride conversion on electrochemical CO2 reduction via in-situ transmission electron microscopy and diffraction
The evolution of Pd-based material during CO2 electroreduction requires further investigation. Here the authors use in-situ liquid-phase transmission electron microscopy and select area diffraction characterization techniques to visualize the morphological and phase structure evolution of the Pd/PdHx catalysts under CO2 electroreduction conditions.
- Ahmed M. Abdellah
- , Fatma Ismail
- & Drew Higgins
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Article
| Open AccessExperimentally validated design principles of heteroatom-doped-graphene-supported calcium single-atom materials for non-dissociative chemisorption solid-state hydrogen storage
Via the first-principles calculations and experimental verifications, a guiding principle is established to design heteroatom-doped-graphene-supported Ca single-atom carbon nanomaterials for efficient non-dissociative solid-state hydrogen storage.
- Yong Gao
- , Zhenglong Li
- & Hongge Pan
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Article
| Open AccessFlexible power generators by Ag2Se thin films with record-high thermoelectric performance
Flexible Ag2Se possesses promising near-room-temperature thermoelectric performance, while trade-off in thermoelectric performance and flexibility enhances its practical utility. Here, the authors fabricate polycrystalline Ag2Se-based thin film with a high ZT of 1.27 at 363 K by Te doping.
- Dong Yang
- , Xiao-Lei Shi
- & Zhi-Gang Chen
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Article
| Open AccessA rechargeable Ca/Cl2 battery
The development of practical Ca metal batteries has been hindered by the cathode chemistry. Here, the authors report a rechargeable Ca/Cl2 battery, which involves the reversible cathode redox reaction between CaCl2 and Cl2.
- Shitao Geng
- , Xiaoju Zhao
- & Hao Sun
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Article
| Open AccessMask-inspired moisture-transmitting and durable thermochromic perovskite smart windows
Thermochromic perovskite smart windows require humidity for operation, but too much can lead to degradation. Tso and coworkers demonstrate a mask-inspired system for humidity regulation, to extend lifespan and minimize optical haze.
- Sai Liu
- , Yang Li
- & Chi Yan Tso
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Article
| Open AccessSustainable biomimetic solar distillation with edge crystallization for passive salt collection and zero brine discharge
Conventional desalination processes generate clean water and reject brine to sea, which is harmful to the aquatic life. Here, the authors propose a low- cost scalable and foldable mangrove-mimetic device for solar thermal distillation and passive salt collection without brine discharge.
- Mohamed A. Abdelsalam
- , Muhammad Sajjad
- & TieJun Zhang
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Article
| Open AccessHighly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia
Inexpensive iron catalysts often exhibit low activity in ammonia decomposition due to a strong iron-nitrogen binding energy. Here the authors demonstrate that combining iron with cobalt to form a Fe-Co bimetallic catalyst overcomes this limitation, presenting a promising solution for enhancing ammonia decomposition efficiency.
- Shilong Chen
- , Jelena Jelic
- & Malte Behrens
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Article
| Open AccessDefect passivation in methylammonium/bromine free inverted perovskite solar cells using charge-modulated molecular bonding
Molecular passivation is promising for improving the performance and operation stability of perovskite solar cells. Here, authors employ piperazine dihydriodide to strengthen adhesion to MA-free perovskite via −NH2I and Mulliken charge distribution, realizing charge-regulated molecular passivation.
- Dhruba B. Khadka
- , Yasuhiro Shirai
- & Kenjiro Miyano
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Article
| Open AccessEffect of solid-electrolyte pellet density on failure of solid-state batteries
A critical challenge of solid-state batteries is Li-filament penetration. Here, by quantifying microstructural properties and employing modeling techniques, the authors provide insight into solid-state battery failure modes and offer design guidelines to enhance safety and performance.
- Mouhamad S. Diallo
- , Tan Shi
- & Gerbrand Ceder
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Article
| Open AccessCatalytic carbon–carbon bond cleavage in lignin via manganese–zirconium-mediated autoxidation
Efforts to produce aromatic monomers through catalytic lignin depolymerization were focused on aryl–ether bond cleavage, while the carbon–carbon bonds of a large fraction of aromatic monomers in lignin are difficult to cleave. Here, the authors report a catalytic autoxidation method using manganese and zirconium salts as catalysts to cleave the C–C bonds in lignin-derived dimers and oligomers from pine and poplar.
- Chad T. Palumbo
- , Nina X. Gu
- & Gregg T. Beckham
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Article
| Open AccessBoosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
Li–CO2 batteries following Li2CO3-product route suffers from low output voltage and severe parasitic reactions. Here, the authors introduce a copper-based solid redox mediator in Li–CO2 batteries with an efficient Li2C2O4 product route to circumvent the shuttle effect and sluggish kinetics caused by soluble mediators.
- Wei Li
- , Menghang Zhang
- & Haoshen Zhou
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Article
| Open AccessModeling critical thermoelectric transports driven by band broadening and phonon softening
The authors develop a quantitative theory to model and tune the electrical transports during critical phase transitions by incorporating both the band broadening effect and carrier-soft TO phonon interactions.
- Kunpeng Zhao
- , Zhongmou Yue
- & Xun Shi
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Article
| Open AccessDown-selection of biomolecules to assemble “reverse micelle” with perovskites
Introducing biomaterials into semiconductors to manifest bio-mimetic functionality is impactful to trigger new enhancement mechanisms. Here, the authors utilize different types of biomolecules to regulate the perovskite crystal lattice and endow a mechanism for stabilizing the metastable lattice.
- Haodong Wu
- , Yuchen Hou
- & Kai Wang
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Article
| Open AccessAn extended substrate screening strategy enabling a low lattice mismatch for highly reversible zinc anodes
The growth of dendrites and the occurrence of side reactions at zinc anodes currently impede the practical use of aqueous zinc batteries. Here, the authors present an advanced substrate screening approach aimed at stabilizing zinc anodes, thereby enabling the development of high-rate zinc-metal batteries.
- Zhiyang Zheng
- , Xiongwei Zhong
- & Guangmin Zhou
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Article
| Open AccessAqueous amine enables sustainable monosaccharide, monophenol, and pyridine base coproduction in lignocellulosic biorefineries
Utilization of the entire lignocellulose is essential for sustainable and cost-effective biorefineries, but it is hindered by a trade-off between efficient carbohydrate utilization and lignin-to-chemical conversion yield. Here, the authors report a mild lignocellulosic fractionation process using aqueous diethylamine which produces a carbohydrate fraction susceptible to enzymatic hydrolysis and a high-quality lignin that delivers high monomer yields upon catalytic amination and depolymerization.
- Li Xu
- , Meifang Cao
- & Xueqing Qiu
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Article
| Open AccessEngineering metal-carbide hydrogen traps in steels
Understanding how hydrogen embrittles steels and developing the solutions are crucial for enabling the hydrogen economy. Here, the authors report a materials design strategy that can increase the hydrogen trapping capacity by creating carbon vacancies in metal carbide precipitates via microalloying.
- Pang-Yu Liu
- , Boning Zhang
- & Yi-Sheng Chen