Featured
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Article
| Open AccessVersatile strategy for homogeneous drying patterns of dispersed particles
Coating technologies call for effective methods capable of suppressing the coffee-ring effect for a uniform particle deposition. Rey et al. show homogeneous drying patterns can be achieved via physically adsorbing polymers onto particle surfaces and the method is applicable to a wide range of materials regardless of the shape of the dispersed particles.
- Marcel Rey
- , Johannes Walter
- & Nicolas Vogel
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Article
| Open AccessAddressing the quantitative conversion bottleneck in single-atom catalysis
The practical application of single atom catalyst (SAC) in liquid-phase heterogeneous catalysis is hampered by the productivity bottleneck as well as catalyst leaching. Here, a bench-top, fast-flow reactor integrated with Pt1-MoS2 SAC was fabricated for continuous production of multifunctional anilines (28 examples) at a record productivity of 5.8 g h-1.
- Zhongxin Chen
- , Jingting Song
- & Kian Ping Loh
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Article
| Open AccessMultimodal confined water dynamics in reverse osmosis polyamide membranes
Polymeric membranes are extensively used in water desalination, but the effect of membrane nanostructure on water transport is still elusive. The authors, using quasi-elastic neutron scattering and contrast variation techniques, provide detailed insight into the dynamics of the polymer network and confined water across a wide range of length and timescales.
- Fabrizia Foglia
- , Bernhard Frick
- & João T. Cabral
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Article
| Open AccessSteering the reaction pathway of syngas-to-light olefins with coordination unsaturated sites of ZnGaOx spinel
Great progress has been made in the development of bifunctional oxide-zeolite catalysts to tackle the selectivity challenge in syngas chemistry. Here the authors show syngas conversion can be steered along a highly active and selective pathway towards light olefins via ketene acetate (acetyl) intermediates.
- Na Li
- , Yifeng Zhu
- & Xinhe Bao
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Article
| Open AccessBreaking scaling relationships in alkynol semi-hydrogenation by manipulating interstitial atoms in Pd with d-electron gain
Circumventing the linear scaling relationship in the semi-hydrogenation is challenging. Here the authors report a method for breaking the scaling relationships using ordered mesoporous carbon-supported Pd nanocatalysts with d-electron gain by p-block atoms occupying interstitial sites in the lattice as a greener alternative to Lindlar catalysts for the selective hydrogenation of alkynols.
- Yang Yang
- , Xiaojuan Zhu
- & Ying Wan
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Article
| Open AccessChiral emergence in multistep hierarchical assembly of achiral conjugated polymers
Chiral assembly of achiral building blocks can engender properties without resorting to complex stereochemistry. Here, the authors reveal chiral emergence from achiral semiconducting polymers which pave the way to chiral (opto)electronics.
- Kyung Sun Park
- , Zhengyuan Xue
- & Ying Diao
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Article
| Open AccessUnderstanding the complementarities of surface-enhanced infrared and Raman spectroscopies in CO adsorption and electrochemical reduction
Infrared and Raman spectroscopies are often assumed to provide similar insights into heterogeneous reaction mechanisms. This study shows that these techniques provide similar data when CO is strongly bound to a surface, yet distinct subpopulations of CO are probed when binding is weaker.
- Xiaoxia Chang
- , Sudarshan Vijay
- & Bingjun Xu
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Article
| Open AccessRecyclable cooperative catalyst for accelerated hydroaminomethylation of hindered amines in a continuous segmented flow reactor
Flow chemistry enables intensified production of hindered amines. Here the authors present a rapid and reusable catalyst to operate in a segmented flow reactor for olefin hydroaminomethylation to selectively produce hindered amines or enamines.
- Malek Y. S. Ibrahim
- & Milad Abolhasani
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Article
| Open AccessAmbient-pressure hydrogenation of CO2 into long-chain olefins
The conversion of CO2 by renewable power-generated hydrogen is a promising approach to a sustainable production of long-chain olefins. Here the authors report a Cu-Fe catalyst which achieves the hydrogenation of CO2 into long-chain olefins under ambient pressure via the synergy of carbide mechanism and CO insertion mechanism.
- Zhongling Li
- , Wenlong Wu
- & Jie Zeng
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Article
| Open AccessA cost-effective alkaline polysulfide-air redox flow battery enabled by a dual-membrane cell architecture
Polysulfide-air redox flow batteries are an appealing energy storage technology but suffer from polysulfide crossover and the use of costly catalysts. Here, the authors report a cell structure that enables battery operation using a cost-effective catalyst while mitigating polysulfide crossover.
- Yuhua Xia
- , Mengzheng Ouyang
- & Nigel P. Brandon
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Article
| Open AccessVertically stacked, low-voltage organic ternary logic circuits including nonvolatile floating-gate memory transistors
High-density information processing without increasing the circuit complexity is highly desired in electronics. Here, Im et al. demonstrate a low-voltage organic ternary logic circuit vertically integrated with the nonvolatile flash memory, increasing the information density by a factor of 3.
- Junhwan Choi
- , Changhyeon Lee
- & Sung Gap Im
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Article
| Open AccessSolid surface frustrated Lewis pair constructed on layered AlOOH for hydrogenation reaction
Designing heterogeneous solid surface frustrated Lewis pair (ssFLP) catalyst for hydrogenation is a new challenge in catalysis. Here, the authors show the ssFLP can be constructed on layered AlOOH for hydrogenation reactions under mild conditions.
- Shulin Liu
- , Minghua Dong
- & Buxing Han
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Article
| Open AccessScalable production of ultrafine polyaniline fibres for tactile organic electrochemical transistors
Strong, electroactive and ultrafine conducting polymer fibres are prepared at the large scale by a modified wet spinning strategy. The obtained ultrafine polyaniline fibres are qualified to build tactile organic electrochemical transistors.
- Bo Fang
- , Jianmin Yan
- & Xiaoming Tao
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Article
| Open AccessLow energy carbon capture via electrochemically induced pH swing with electrochemical rebalancing
This work demonstrates a safe and scalable electrochemical CO2 separation method that allows promisingly low (62 kJ/molCO2) energetic cost at a high current density, and it can be used for direct air capture when a suitable molecule is used.
- Shijian Jin
- , Min Wu
- & Michael J. Aziz
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Article
| Open AccessChirality transfer from a 3D macro shape to the molecular level by controlling asymmetric secondary flows
External physical forces can bias a spontaneous symmetry breaking process but whether the shape of a reactor plays a role in chiral symmetry breaking processes is an open question. Here, the authors demonstrate chirality transfer from the chiral shape of a 3D helical channel to chiral supramolecular aggregates whereby the handedness of the helical channel dictates the direction of enantioselection.
- Semih Sevim
- , Alessandro Sorrenti
- & Josep Puigmartí-Luis
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Article
| Open AccessHigh-speed 4D neutron computed tomography for quantifying water dynamics in polymer electrolyte fuel cells
Characterisation of water dynamics in polymer electrolyte fuel cells is important for technology development. Here, the authors demonstrate a 4D neutron imaging technique, enabling quantitative analysis of the local water evolution, and identify performance parameters for water management.
- Ralf F. Ziesche
- , Jennifer Hack
- & Paul R. Shearing
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Article
| Open AccessHydrogen spillover assisted by oxygenate molecules over nonreducible oxides
Spontaneous migration of H-atoms from metal particles to a nonreducible oxide support is generally limited by thermodynamics. Here, small oxygenate molecules are found to act as effective H-carriers to promote this process and lead to much improved hydrodeoxygenation rates on Pt-Fe/SiO2 catalysts.
- Mingwu Tan
- , Yanling Yang
- & Yong Wang
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Article
| Open AccessControl of zeolite framework flexibility for ultra-selective carbon dioxide separation
All-silica zeolite membranes are highly desired for natural gas upgrading but the size-exclusion effect is compromised by defects generated during high-temperature detemplation. Here, the authors develop a strategy to fabricate ultra-selective DD3R zeolite membranes via tuning the zeolite flexibility under rapid template decomposition.
- Peng Du
- , Yuting Zhang
- & Xuehong Gu
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Article
| Open AccessTrends in oxygenate/hydrocarbon selectivity for electrochemical CO(2) reduction to C2 products
Key mechanistic steps for selective CO(2) reduction over Cu into hydrocarbon versus oxygenated C2 products are identified by atomistic and microkinetic modeling. Variations in C and OH binding are found to predict catalytic selectivity of materials.
- Hong-Jie Peng
- , Michael T. Tang
- & Frank Abild-Pedersen
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Article
| Open AccessOxo dicopper anchored on carbon nitride for selective oxidation of methane
Selective conversion of methane into value-added chemicals is a promising approach for utilization of hydrocarbon sources. Here the authors develop dimeric copper centers supported on graphitic carbon nitride (denoted as Cu2@C3N4) with >10% conversion and >98% selectivity toward methyl oxygenates in both thermo- and photo- catalytic reactions.
- Pengfei Xie
- , Jing Ding
- & Chao Wang
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Article
| Open AccessA high-performance capillary-fed electrolysis cell promises more cost-competitive renewable hydrogen
Water electrolysis offers a promising means for green hydrogen production, however current electrolysers do not provide a competitive edge over fossil fuels. Here, authors develop a capillary-fed electrolyser setup that avoids bubble formation to achieve a high-performance, cost-competitive device.
- Aaron Hodges
- , Anh Linh Hoang
- & Gordon G. Wallace
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Article
| Open AccessEngineered assembly of water-dispersible nanocatalysts enables low-cost and green CO2 capture
Catalytic solvent regeneration is of interest to reduce energy consumption in CO2 separation, however, the development of engineered nanocatalysts remains a challenge. Here, a new avenue is presented for the next generation of advanced metal-organic frameworks (MOFs) in energy-efficient CO2 capture.
- Masood S. Alivand
- , Omid Mazaheri
- & Kathryn A. Mumford
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Article
| Open AccessHigh drug-loaded microspheres enabled by controlled in-droplet precipitation promote functional recovery after spinal cord injury
High drug loading improves therapeutic efficacy and reduces side effects in drug delivery. Here, the authors use controlled diffusion of solvents to precipitate drug nanoparticles in polymer particles while the polymer is solidifying and demonstrate the particles for drug delivery in a spinal cord injury model.
- Wei Li
- , Jian Chen
- & Dongfei Liu
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Comment
| Open AccessAutonomous platforms for data-driven organic synthesis
Achieving autonomous multi-step synthesis of novel molecular structures in chemical discovery processes is a goal shared by many researchers. In this Comment, we discuss key considerations of what an ideal platform may look like and the apparent state of the art. While most hardware challenges can be overcome with clever engineering, other challenges will require advances in both algorithms and data curation.
- Wenhao Gao
- , Priyanka Raghavan
- & Connor W. Coley
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Article
| Open AccessIn-situ transfer vat photopolymerization for transparent microfluidic device fabrication
Despite many advantages of vat photopolymerization in microfluidic device fabrication, well-controlled μm-sized (< 100 μm) channels in the layer building direction remains a challenge. Here, authors present a general high resolution and low-cost 3D printing process that can produce devices within the 10 μm scale.
- Yang Xu
- , Fangjie Qi
- & Yong Chen
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Article
| Open AccessAtomically unveiling the structure-activity relationship of biomacromolecule-metal-organic frameworks symbiotic crystal
Biomolecule-metal-organic-frameworks allow for the creation of hybrid materials with desired biological and chemical function. Here, the authors refine the structure-function relationship by identifying the atomic-layer structure of the hybrids and show differences in structure upon different crystallisation pathways.
- Linjing Tong
- , Siming Huang
- & Gangfeng Ouyang
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Article
| Open AccessPartially sintered copper‒ceria as excellent catalyst for the high-temperature reverse water gas shift reaction
Constructing stable active sites in catalysts for high temperature catalytic reactions remains challenging. Here, the authors manage to make stable copper clusters in the copper‒ceria catalyst with high Cu loading (15 wt.%) for the high-temperature reverse water gas shift reaction.
- Hao-Xin Liu
- , Shan-Qing Li
- & Chun-Jiang Jia
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Article
| Open AccessPolyamide-based membranes with structural homogeneity for ultrafast molecular sieving
Thin-film composite membranes formed by conventional interfacial polymerization generally suffer from depth heterogeneity of the polyamide layer. Here, authors investigate salt-mediated polymerization approaches to achieve membranes with tuneable structural homogeneity.
- Liang Shen
- , Ruihuan Cheng
- & Yan Wang
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Article
| Open AccessObservation and rationalization of nitrogen oxidation enabled only by coupled plasma and catalyst
Heterogeneous catalysts coupled with non-thermal plasma are known to achieve higher reaction yields, but disentangling the gain achieved by the individual components remains challenging. Here, NO is produced from N2 and O2 in a plasma-catalytic reactor at conditions at which neither catalyst nor plasma alone is productive, providing unambiguous evidence of plasma-catalyst synergy.
- Hanyu Ma
- , Rakesh K. Sharma
- & William F. Schneider
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Article
| Open AccessManipulation and control of droplets on surfaces in a homogeneous electric field
Control of droplet coalescence is a major challenge of droplet microfluidics. Here, the authors show that homogenous external electric field can induce dipoles inside droplets, which can be used to withdraw samples from an array of droplets.
- Johannes Hartmann
- , Maximilian T. Schür
- & Steffen Hardt
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Article
| Open AccessCatalytic production of low-carbon footprint sustainable natural gas
The recalcitrance of lignocellulosic biomass is the major limitation for the production of natural gas. Here the authors develop a catalytic-drive approach with Ni2Al3 alloy catalyst to enable nearly complete conversion of various agricultural and forestry residues into natural gas.
- Xiaoqin Si
- , Rui Lu
- & Fang Lu
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Article
| Open AccessRobust ultrathin nanoporous MOF membrane with intra-crystalline defects for fast water transport
The development of highly water-permeable membranes is key for the treatment of high salinity waters. Here the authors enhance the water permeability of a metal-organic framework nanoporous membrane via an intra-crystalline defect engineering strategy.
- Xueling Wang
- , Qiang Lyu
- & Yingchao Dong
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Article
| Open AccessEnhanced hydrogen generation by reverse spillover effects over bicomponent catalysts
H2 is regarded as an attractive green fuel and a promising energy carrier for the future. Here, the promotion functions of reverse spillover effects in the H2 generation reactions over bicomponent catalysts are revealed by performing in situ X ray absorption near edge structure characterization.
- Zhe Gao
- , Guofu Wang
- & Yong Qin
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Article
| Open AccessEngineering immunomodulatory and osteoinductive implant surfaces via mussel adhesion-mediated ion coordination and molecular clicking
Immune response and new tissue formation are important aspects of tissue repair but often only one aspect is considered in biomedical interventions. Here, the authors report on the use of a mussel-like surface coating to immobilize immune modulating metal ions and growth factors and demonstrated improved in vivo outcomes.
- Tao Wang
- , Jiaxiang Bai
- & Lianfu Deng
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Article
| Open AccessUltra-high thermal stability of sputtering reconstructed Cu-based catalysts
Applications of Cu catalysts at high-temperature is a long-sought goal but limited by their serious deactivation due to low copper’s Tammann temperature. Here, the authors introduce an encapsulation layer to improve thermal stability at 800 °C by reconstructing electronic structure of Cu atoms.
- Jiafeng Yu
- , Xingtao Sun
- & Jian Sun
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Article
| Open AccessAugmenting zero-Kelvin quantum mechanics with machine learning for the prediction of chemical reactions at high temperatures
Computational material design often does not account for temperature effects. The present manuscript combines quantum-mechanics based calculations with a machine-learned correction to establish a unified thermodynamics framework for accurate prediction of high temperature reaction free energies in oxides.
- Jose Antonio Garrido Torres
- , Vahe Gharakhanyan
- & Alexander Urban
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Article
| Open AccessSelective cobalt and nickel electrodeposition for lithium-ion battery recycling through integrated electrolyte and interface control
Recovery of metals from Li-ion batteries is a key for sustainability. Here the authors demonstrate a Li-ion cell recycling process via selective electrochemical Co and Ni recovery by controlling the electrode interface and the electrolyte.
- Kwiyong Kim
- , Darien Raymond
- & Xiao Su
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Article
| Open AccessSelf-wetting triphase photocatalysis for effective and selective removal of hydrophilic volatile organic compounds in air
Photocatalytic air purification is promising but it calls for more efficient photocatalytic materials and systems. Here, the authors report a strategy to introduce an in-situ water layer on WO3 by coating hygroscopic periodic acid that effectively remove hydrophilic volatile organic compounds.
- Fei He
- , Seunghyun Weon
- & Wonyong Choi
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Article
| Open AccessThe origin of the particle-size-dependent selectivity in 1-butene isomerization and hydrogenation on Pd/Al2O3 catalysts
The selectivity of Pd catalysts in 1-butene hydrogenation and isomerization depends on nanoparticle size. Herein, the authors show by combining experiment and modeling that the type and specific properties of the contributing surface facets are decisive for the selectivity.
- Alexander Genest
- , Joaquín Silvestre-Albero
- & Günther Rupprechter
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Article
| Open AccessEvolution of the electronic structure in open-shell donor-acceptor organic semiconductors
The classical narrow bandgap donor-acceptor organic semiconductors show great application potential in organic electronics, bio-imaging and other fields. Here, the authors systematically and rigorously demonstrate their open-shell diradical character via experimental and theoretical investigation.
- Zhongxin Chen
- , Wenqiang Li
- & Fei Huang
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Article
| Open AccessGrafting nanometer metal/oxide interface towards enhanced low-temperature acetylene semi-hydrogenation
Metal/oxide interface is of fundamental significance to heterogeneous catalysis. Here, the authors construct a nanometer Pd/Bi2O3 interface by grafting Pd clusters onto Bi2O3 clusters and demonstrate its essential roles in the low-temperature semi-hydrogenation of acetylene.
- Shihui Zou
- , Baohui Lou
- & Jie Fan
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Article
| Open AccessTunable and functional deep eutectic solvents for lignocellulose valorization
Deep eutectic solvents (DES) are intriguing green reaction media for biomass processing, however, undesired lignin condensation is a typical drawback. Here the authors develop a tunable ternary DES system that allows for stabilization of reactive intermediates for efficient lignocellulose fractionation.
- Yongzhuang Liu
- , Noemi Deak
- & Katalin Barta
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Article
| Open AccessNear 100% ethene selectivity achieved by tailoring dual active sites to isolate dehydrogenation and oxidation
It is important but challenging to prohibit deep oxidation of alkene in oxidative dehydrogenation of light alkane. Here, dual active sites are tailored to isolate dehydrogenation and oxidation thus achieving superior ethene selectivity.
- Chaojie Wang
- , Bing Yang
- & Xiaodong Wang
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Article
| Open AccessLight-fueled transient supramolecular assemblies in water as fluorescence modulators
Dissipative self-assembly, which requires a continuous supply of fuel to maintain the assembled states far from equilibrium, is the foundation of biological systems but it remains a challenge to introduce light as fuel into artificial dissipative self-assemblies. Here, the authors report an artificial dissipative self-assembly system that is constructed from light-induced amphiphiles.
- Xu-Man Chen
- , Xiao-Fang Hou
- & Quan Li
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Article
| Open AccessEfficiency and selectivity of CO2 reduction to CO on gold gas diffusion electrodes in acidic media
Large scale CO2 electrolysis to produce CO has mainly been performed in neutral and alkaline media. Here, we show that it can also be realized in acidic media, with faradaic efficiencies of 80–90%, and 30% better energy efficiency than obtained in neutral media.
- Mariana C. O. Monteiro
- , Matthew F. Philips
- & Marc T. M. Koper
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Article
| Open AccessZn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds
Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Here, the authors report that Zn2+ coordinated with N species on N-doped carbon catalysts can catalyze the aerobic oxidative cleavage and esterification of C(CO)-C bonds with high efficiency and activity.
- Chao Xie
- , Longfei Lin
- & Buxing Han
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Article
| Open AccessA cost-effective and humidity-tolerant chloride solid electrolyte for lithium batteries
Stable inorganic solid electrolytes are instrumental in developing high-voltage Li metal batteries. Here, the authors present the synthesis and electrochemical energy storage properties of a cost-effective and humidity-tolerant chloride solid electrolyte.
- Kai Wang
- , Qingyong Ren
- & Cheng Ma
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Article
| Open AccessEvanescent waves modulate energy efficiency of photocatalysis within TiO2 coated optical fibers illuminated using LEDs
Coupling photocatalyst-coated optical fibers (P-OFs) with LEDs shows potential in environmental applications. Here the authors report a strategy to maximize P-OF light usage and simultaneously establish a new platform to quantify photocatalytic performance.
- Yinghao Song
- , Li Ling
- & Chii Shang
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Article
| Open AccessTransforming biorefinery designs with ‘Plug-In Processes of Lignin’ to enable economic waste valorization
The current biorefineries yield lignin with inadequate fractionation for bioconversion, yet substantial changes of these biorefinery designs could jeopardize carbohydrate efficiency and increase capital costs. Here the authors resolve the dilemma by designing ‘plug-in processes of lignin’ to enable economic waste valorization.
- Zhi-Hua Liu
- , Naijia Hao
- & Joshua S. Yuan