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| Open AccessTautomerism unveils a self-inhibition mechanism of crystallization
Modifiers of diverse materials exhibit structures or compositions that differ from a solute molecule but often contain similar functional motifs that facilitate molecular recognition for modifier binding to crystal surfaces. Here the authors examine the intrinsic capability of tautomers, or structural isomers, to operate as crystal growth inhibitors.’
- Weiwei Tang
- , Taimin Yang
- & Jeffrey D. Rimer
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Article
| Open AccessZhang-Rice singlets state formed by two-step oxidation for triggering water oxidation under operando conditions
The Zhang-Rice singlet is known for the superconductivity of high-temperature superconductors cuprate but is rarely studied for an electrochemical catalyst. Here, the authors use operando spectroscopic tools and observe Cu active site evolves into high-valent CuO4 geometry with Cu3+ active species, so-called Zhang-Rice singlet state, during oxygen evolution reaction.
- Chun-Kuo Peng
- , Yu-Chang Lin
- & Yan-Gu Lin
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Article
| Open AccessBenchmark single-step ethylene purification from ternary mixtures by a customized fluorinated anion-embedded MOF
Ethylene (C2H4) purification from multi-component mixtures by physical adsorption is a great challenge in the chemical industry. Here authors present a GeF62- anion embedded MOF ZNU-6 with customized pore structure and pore chemistry for benchmark one-step C2H4 recovery from C2H2 and CO2 with record C2H4 productivity.
- Yunjia Jiang,
- , Yongqi Hu,
- & Yuanbin Zhang
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Article
| Open AccessElectrochemical direct air capture of CO2 using neutral red as reversible redox-active material
Electrochemical direct air capture (DAC) of CO2 requires air-stable redox-active materials. Here, the authors present an electrochemical DAC using air-stable redox couple of neutral red with a minimum energy requirement of 65 kJe/molCO2.
- Hyowon Seo
- & T. Alan Hatton
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Article
| Open AccessAn iron-base oxygen-evolution electrode for high-temperature electrolyzers
A low-cost and efficient high-temperature oxygen evolution reaction electrode is a big challenge. Here, the authors report an iron-base electrode with an in situ formed lithium ferrite for enhanced stability and catalytic activity in molten carbonate and chloride salts and achieve kiloampere-scale electrolysis.
- Kaifa Du
- , Enlai Gao
- & Dihua Wang
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Article
| Open AccessIon sieving in graphene oxide membrane enables efficient actinides/lanthanides separation
Separation of actinides from lanthanides is very important for the safe management of nuclear waste, however still challenging due to the chemical complexity of the f-elements. Here, authors report an efficient strategy with graphene oxide membranes for ion sieving of high valent actinyl ions and spherical lanthanide ions.
- Zhipeng Wang
- , Liqin Huang
- & Chao Xu
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Article
| Open AccessPorous organic polycarbene nanotrap for efficient and selective gold stripping from electronic waste
Efficient and selective gold recovery from electronic waste is highly demanded. Here, authors demonstrate the application of a porous organic polycarbene adsorbent with up to 2.09 g/g gold-capturing capability.
- Xinghao Li
- , Yong-Lei Wang
- & Yaozu Liao
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Article
| Open AccessPt nanoclusters on GaN nanowires for solar-asssisted seawater hydrogen evolution
Seawater is the most abundant water source for hydrogen fuel production. Here the authors report a binary photoelectrode of Pt catalyst-GaN semiconductor with promising efficiency, productivity, and stability for seawater hydrogen evolution.
- Wan Jae Dong
- , Yixin Xiao
- & Zetian Mi
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Article
| Open AccessGreen synthesis of propylene oxide directly from propane
Propylene and propylene oxide are formed over boron nitride or SiO2 in the gas phase without yielding large amounts of CO2. Conversion at non-specific interfaces can thus be a successful strategy for the synthesis of oxidation-sensitive products.
- Pierre Kube
- , Jinhu Dong
- & Annette Trunschke
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Article
| Open AccessGradient area-selective deposition for seamless gap-filling in 3D nanostructures through surface chemical reactivity control
Integrating bottom-up and top-down fabrication techniques can overcome limits in nanofabrication. Here authors demonstrate an approach for area selective deposition using Ti as an inhibitor in the atomic layer deposition process to achieve controlled growth of seamless TiO2 layers on 3D structures.
- Chi Thang Nguyen
- , Eun-Hyoung Cho
- & Han-Bo-Ram Lee
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Article
| Open AccessAn embedded interfacial network stabilizes inorganic CsPbI3 perovskite thin films
Lattice anchoring, in its varied forms, has proven effective at regulating the energetics of metastable phases of polymorphic crystals. Here, the authors utilize top-down photolithography to embed a tessellating 3D interfacial network into otherwise-unstable CsPbI3 perovskite thin films and devices, stabilizing the perovskite phase.
- Julian A. Steele
- , Tom Braeckevelt
- & Maarten B. J. Roeffaers
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Article
| Open AccessToward economical application of carbon capture and utilization technology with near-zero carbon emission
Carbon capture, utilization and storage technology is limited by the need for a separate CO2 capture step. Here, the authors propose a strategy and economic analysis for simultaneous dilute CO2 capture from flue gas and direct electrochemical reduction to synthesis gas via reaction swing absorption.
- Kezia Megagita Gerby Langie
- , Kyungjae Tak
- & Ung Lee
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Article
| Open AccessAntifouling graphene oxide membranes for oil-water separation via hydrophobic chain engineering
Fouling is a continuous challenge for the effective application of membranes in oily wastewater treatment. Here, the authors present a hydrophobic chain engineering strategy to regulate the surface of graphene oxide-based membranes at a molecular scale for increased antifouling even at high permeance.
- Chao Yang
- , Mengying Long
- & Zhongyi Jiang
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Article
| Open AccessRapid atom-efficient polyolefin plastics hydrogenolysis mediated by a well-defined single-site electrophilic/cationic organo-zirconium catalyst
Polyolefins are a major fraction of plastic waste, yet their catalytic recycling is challenging due to their inert hydrocarbon structures. Here a well-defined supported organozirconium catalyst is shown to mediate the rapid hydrogenolytic cleavage diverse polyolefins under very mild conditions.
- Alexander H. Mason
- , Alessandro Motta
- & Tobin J. Marks
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Article
| Open AccessBack-illuminated photoelectrochemical flow cell for efficient CO2 reduction
Conversion of CO2 into value-added products with renewable energy provides a promising route to realize carbon neutrality. Here, authors design and construct a Si photoelectrochemical flow cells for CO2 reduction reaction to achieve a high solar-to-fuel conversion efficiency.
- Bin Liu
- , Tuo Wang
- & Jinlong Gong
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| Open AccessBoosting CO hydrogenation towards C2+ hydrocarbons over interfacial TiO2−x/Ni catalysts
Considerable attention has been drawn to tune the geometric and electronic structure of interfacial catalysts via modulating strong metal-support interactions (SMSI). Here the authors report the remarkable catalytic performance of CO hydrogenation over an interfacial TiO2−x/Ni catalyst by means of SMSI.
- Ming Xu
- , Xuetao Qin
- & Ding Ma
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Article
| Open AccessSpheroplasts preparation boosts the catalytic potential of a squalene-hopene cyclase
Squalene-hopene cyclase are membrane-bound enzymes used to produce bioactive compounds at industrial scale. Here, the authors show squalene-hopene cyclase spheroplasts, obtained by removing the outer cell membrane, having a higher catalytic activity than the enzymes and the whole cells, and their cross-linking for recycling and reuse.
- Ana I. Benítez-Mateos
- , Andreas Schneider
- & Francesca Paradisi
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Article
| Open AccessMembrane-based TBADT recovery as a strategy to increase the sustainability of continuous-flow photocatalytic HAT transformations
Decatungstate-enabled Hydrogen Atom Transfer (HAT) photocatalysis of hydrocarbon scaffolds enabled rapid access to new C(sp3)-enriched chemical space. Here, the authors present in-line TBADT recovery with organic solvent nanofiltration (OSN) as an answer to the concerns surrounding the scale-up of decatungstate HAT reactions, i.e., catalyst loading and cost.
- Zhenghui Wen
- , Diego Pintossi
- & Timothy Noël
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| Open AccessHigh-resolution neutron imaging of salt precipitation and water transport in zero-gap CO2 electrolysis
The electrochemical reduction of CO2 is pivotal for the chemical industry to reach climate neutrality. Here, the authors utilize high-resolution neutron imaging to unravel electrode flooding and salt precipitation, both major hurdles to steady operation of CO2 electrolyzers.
- Joey Disch
- , Luca Bohn
- & Severin Vierrath
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Article
| Open AccessEmergent microrobotic oscillators via asymmetry-induced order
Spontaneous low-frequency oscillations, which are a feature of biological systems, are challenging to engineer into microrobotic systems. The authors discover a mechanism for asymmetry-induced order and realise electrical and mechanical oscillations in a particle collective to power a microrobotic arm.
- Jing Fan Yang
- , Thomas A. Berrueta
- & Michael S. Strano
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Article
| Open AccessDirect production of olefins from syngas with ultrahigh carbon efficiency
Zhong et al report sodium-promoted metallic Ru nanoparticles for the direct production of olefins from syngas with ultrahigh carbon efficiency where the total selectivity of undesired CH4 and CO2 is suppressed to only 5% for over 500 hours on stream.
- Hailing Yu
- , Caiqi Wang
- & Liangshu Zhong
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Article
| Open AccessA supraparticle-based biomimetic cascade catalyst for continuous flow reaction
Robust millimeter-sized spherical particles with controlled compositions and microstructures hold promises of important practical applications. Here the authors develop a liquid marble method to facilely fabricate robust millimeter-sized supraparticles with controlled microstructures through the bottom-up assembly of silica nanoparticles.
- Xiaomiao Guo
- , Nan Xue
- & Hengquan Yang
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Article
| Open AccessFast hydrogen purification through graphitic carbon nitride nanosheet membranes
In this work, lamellar graphitic carbon nitride nanosheet membranes are constructed for gas separation. Benefiting from their high-density intrinsic in-plane nanopores and broader permeable interlayer channels, the proposed membranes exhibit high H2 permeance with good selectivity of multiple gas mixtures.
- Yisa Zhou
- , Ying Wu
- & Haihui Wang
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Article
| Open AccessCement substitution with secondary materials can reduce annual global CO2 emissions by up to 1.3 gigatons
In this paper we report the maximum potential for cement substitution with secondary materials to reduce CO2 emissions globally (1.3 Gt CO2-eq. in 2018) and on a country-by-country basis.
- Izhar Hussain Shah
- , Sabbie A. Miller
- & Rupert J. Myers
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Article
| Open AccessSynergy of metal nanoparticles and organometallic complex in NAD(P)H regeneration via relay hydrogenation
Homogenous and heterogeneous catalysts were applied separately and rarely catalyzed a target reaction synergistically. Herein, the authors identify the synergy effect of these two types of catalysts in NAD(P)H regeneration via relay hydrogenation.
- Maodi Wang
- , Zhenchao Zhao
- & Qihua Yang
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Article
| Open AccessA hygroscopic nano-membrane coating achieves efficient vapor-fed photocatalytic water splitting
Although light-driven water vapor splitting may avoid material stability challenges for renewable fuel production, material performances lag behind solution-based studies. Here, authors incorporate metal hydroxides layers into particulate photocatalysts to enhance water vapor splitting activities.
- Takuya Suguro
- , Fuminao Kishimoto
- & Kazuhiro Takanabe
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Article
| Open AccessFlame-made ternary Pd-In2O3-ZrO2 catalyst with enhanced oxygen vacancy generation for CO2 hydrogenation to methanol
Assembling multicomponent catalysts to harness synergic effects is challenging. Now, flame spray pyrolysis permits the synthesis of ternary Pd-In2O3-ZrO2 catalysts with an optimal architecture and an enriched density of oxygen vacancies for maximal performance in CO2-based methanol synthesis.
- Thaylan Pinheiro Araújo
- , Cecilia Mondelli
- & Javier Pérez-Ramírez
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| Open AccessAccelerating syngas-to-aromatic conversion via spontaneously monodispersed Fe in ZnCr2O4 spinel
Spontaneous monodispersion of active species and their stabilization in reductive atmospheres remain a challenge in catalytic syngas chemistry. Here the authors demonstrate that syngas-to-aromatic conversion can be significantly accelerated by the spontaneously monodispersed Fe in ZnCr2O4 spinel.
- Guo Tian
- , Xinyan Liu
- & Fei Wei
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Article
| Open AccessSustainable production of hydrogen with high purity from methanol and water at low temperatures
Carbon neutrality initiative has stimulated the development of the sustainable methodologies for hydrogen generation and safe storage. Here the authors demonstrate that the dual-active sites of Pt single-atoms and frustrated Lewis pairs on porous nanorods of CeO2 enable the efficient additive-free H2 generation with a low CO generation through reforming of methanol and water.
- Sai Zhang
- , Yuxuan Liu
- & Yongquan Qu
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Article
| Open AccessMechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene
Designing atomically uniform ensemble sites for matching targeted reaction pathway is important yet challenging in heterogeneous catalysis. Here, the authors fabricate a trimer Ni1Sb2 site featuring superior selectivity for acetylene semi-hydrogenation via a mechanism-driven design strategy.
- Xiaohu Ge
- , Mingying Dou
- & Xuezhi Duan
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Article
| Open AccessPt1 enhanced C-H activation synergistic with Ptn catalysis for glycerol cascade oxidation to glyceric acid
The selective oxidation of glycerol to glyceric acid is an important value-added cascade catalytic process. Here the authors report a cascade synergistic catalysis strategy by atomic and low-coordinated cluster Pt on well-defined Cu-CuZrOx to simultaneously achieve high activity and selectivity.
- Zhe An
- , Zilong Zhang
- & Jing He
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Article
| Open AccessEnergy comparison of sequential and integrated CO2 capture and electrochemical conversion
Coupling CO2 capture and electrolysis offers new opportunities to reduce energy cost. Here, the authors identify that the integrated electrolyser must show similar performance to the gas-fed electrolyser to ensure an energy benefit of up to 44% versus sequential capture and conversion processes.
- Mengran Li
- , Erdem Irtem
- & Thomas Burdyny
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Article
| Open AccessIdentifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst
The direct electrocatalytic synthesis of urea via C–N coupling is of great significance. The authors report a diatomic catalyst with bonded Fe–Ni pairs to improve the efficiency of electrochemical urea synthesis from nitrate and CO2.
- Xiaoran Zhang
- , Xiaorong Zhu
- & Shuangyin Wang
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Article
| Open AccessTopographic design in wearable MXene sensors with in-sensor machine learning for full-body avatar reconstruction
Wearable sensors with edge computing are desired for human motion monitoring. Here, the authors demonstrate a topographic design for wearable MXene sensor modules with wireless streaming or in-sensor computing models for avatar reconstruction.
- Haitao Yang
- , Jiali Li
- & Po-Yen Chen
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Article
| Open AccessHydrogen production from the air
While obtaining H2 from water splitting offers a promising strategy for renewable fuel production, current technologies rely on liquid freshwater. Here, authors use a hygroscopic electrolyte to achieve electrocatalytic water vapor splitting driven by renewable resources without liquid water.
- Jining Guo
- , Yuecheng Zhang
- & Gang Kevin Li
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Article
| Open AccessSpatiotemporal control of signal-driven enzymatic reaction in artificial cell-like polymersomes
Researchers have been trying to mimick the cellular spatiotemporal control in normal cells with different approaches. Here, the authors present semi-permeable polymersomes comprising of amphiphilic triblock copolymers to achieve external signal-driven complex coacervation and biophysical reconstitution of cytoskeleton.
- Hanjin Seo
- & Hyomin Lee
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Article
| Open AccessPrecursor engineering of hydrotalcite-derived redox sorbents for reversible and stable thermochemical oxygen storage
Thermochemical redox reactions of metal oxides are promising for CO2 capture, gas purification, air separation, and energy storage. Here, the authors report mixed metal oxides derived from layered double hydroxides precursors, and demonstrate their reversible and stable thermochemical oxygen storage.
- Michael High
- , Clemens F. Patzschke
- & Qilei Song
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Article
| Open AccessElectron-mediated control of nanoporosity for targeted molecular separation in carbon membranes
Controlled molecular separation by membranes requires 2D materials with precise structures to achieve the desired selectivity. Here authors demonstrate precise selectivity tuning in carbon membranes using electron irradiation.
- Banseok Oh
- , Hyeokjun Seo
- & Dong-Yeun Koh
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Article
| Open AccessUltramicroporous material based parallel and extended paraffin nano-trap for benchmark olefin purification
Selective paraffin capture to afford high-purity olefins directly is critical but still challenging. Herein, the authors discover a distinctive ultramicroporous material featuring closely packed and linearly-extended isophthalic acid units and thus serving as a paraffin nano-trap for the efficient production of ultra-high purity olefins from paraffins.
- Peixin Zhang
- , Lifeng Yang
- & Huabin Xing
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Article
| Open AccessEnvironmentally adaptive MOF-based device enables continuous self-optimizing atmospheric water harvesting
Atmospheric water harvesting by MOF-based devices is critically dependent on weather conditions. Here, the authors report a MOF-based adaptive water harvesting system capable of adapting its cycles to temperature and relative humidity fluctuations throughout the day, continuously optimizing water production.
- Husam A. Almassad
- , Rada I. Abaza
- & Kyle E. Cordova
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Article
| Open AccessDeep reaction network exploration at a heterogeneous catalytic interface
This study demonstrates how reaction network characterization can be performed on heterogeneous catalytic surfaces predictively, rather than retrospectively, using automated exploration algorithms on an ethylene oligomerization exemplar reaction.
- Qiyuan Zhao
- , Yinan Xu
- & Brett M. Savoie
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Article
| Open AccessHydrogen-bonded organic framework biomimetic entrapment allowing non-native biocatalytic activity in enzyme
Heme units are immobilised in diverse heme enzymes for oxidation, and have been immobilised also in hydrogen-bonded organic frameworks. Here, the authors show the use of hydrogen-bonded organic framework to modulate the enzyme’s conformation and show different biofunction from the original.
- Guosheng Chen
- , Linjing Tong
- & Gangfeng Ouyang
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Article
| Open AccessEfficient separation of butane isomers via ZIF-8 slurry on laboratory- and pilot-scale
The separation of butane isomers, raw materials in petrochemical industry, is challenging. Here the authors report the separation of n-butane and isobutane using a metal-organic framework slurry; the separation can be performed at large scale in a pilot-scale separation tower.
- Mingke Yang
- , Huishan Wang
- & Guangjin Chen
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Article
| Open AccessThe role of solid solutions in iron phosphate-based electrodes for selective electrochemical lithium extraction
Lithium extraction from dilute sources could help solve the lithium supply security issue. Here, the authors investigate the Li- and Na- ion co-intercalation behavior in iron phosphate electrodes and demonstrate the lithium selectivity control through intercalation kinetic manipulations.
- Gangbin Yan
- , George Kim
- & Chong Liu
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Article
| Open AccessHighly efficient and selective extraction of gold by reduced graphene oxide
High extraction capacity with precise selectivity to trace amounts of gold over a wide range of co-existing elements remains a challenge for effective e-waste recycling. Here, authors demonstrate the excellent performance of rGO for gold extraction from e-waste leachate, even at minute concentrations.
- Fei Li
- , Jiuyi Zhu
- & Hui-Ming Cheng
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Article
| Open AccessStable solar water splitting with wettable organic-layer-protected silicon photocathodes
Preparation of inorganic protective layers for photoelectrodes requires high-quality deposition techniques. Here, the authors report a spin-coated organic protective layer that enables Si photocathodes to realize stable solar water splitting.
- Bo Wu
- , Tuo Wang
- & Jinlong Gong
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Article
| Open AccessSpongy all-in-liquid materials by in-situ formation of emulsions at oil-water interfaces
All-in-liquid printing promises applications from energy storage to drug delivery and tissue engineering. Here, authors present the in-situ generation of layered emulsion in a fraction of a second at the oil-water interface forming 3D tube-like structures in a liquid medium.
- Parisa Bazazi
- , Howard A. Stone
- & S. Hossein Hejazi
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Article
| Open AccessBuilding programmable multicompartment artificial cells incorporating remotely activated protein channels using microfluidics and acoustic levitation
Engineering micro-emulsion plays a key role in the creation of bottom-up synthetic cells. Here, authors demonstrate a droplet laboratory platform to control membrane protein gating in functional artificial cell using microfluidics and acoustic levitation.
- Jin Li
- , William D. Jamieson
- & David A. Barrow
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Article
| Open AccessSolvent-driven fractional crystallization for atom-efficient separation of metal salts from permanent magnet leachates
Rare earth elements are essential to electrified infrastructure and clean energy production. Here, authors show reagent- and energy-efficient separation of lanthanides from secondary feedstock using dimethyl ether-driven fractional crystallization.
- Caleb Stetson
- , Denis Prodius
- & Aaron D. Wilson