Featured
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| Open AccessA robust Th-azole framework for highly efficient purification of C2H4 from a C2H4/C2H2/C2H6 mixture
Separation of ethylene from C2 ternary mixture with high working capacity is a challenging task. Here, the authors report a Th-azole framework (Azole-Th-1) for highly efficient purification of ethylene from C2H4/C2H6 and C2H4/C2H2/C2H6 mixtures, respectively.
- Zhenzhen Xu
- , Xiaohong Xiong
- & Banglin Chen
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Article
| Open AccessGeneral route to design polymer molecular weight distributions through flow chemistry
The properties of a polymer are known to be intrinsically related to its molecular weight distribution. Here the authors use a design to synthesis protocol for producing a targeted molecular weight distribution with a computer controlled tubular flow reactor.
- Dylan J. Walsh
- , Devin A. Schinski
- & Damien Guironnet
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Article
| Open AccessDynamic and scalable DNA-based information storage
The physical architectures of information storage dictate how data is encoded, organised and accessed. Here the authors use DNA with a single-strand overhang as a physical address to access specific data and do in-storage file operations in a scalable and reusuable manner.
- Kevin N. Lin
- , Kevin Volkel
- & Albert J. Keung
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Article
| Open AccessSelf-regulating photochemical Rayleigh-Bénard convection using a highly-absorbing organic photoswitch
Autonomous control of liquid motion is vital to the development of new actuators and pumps in fluid systems but autonomous control of fluid motion is inaccessible in current systems. Here, the authors identify unique features of a photochromic molecular switch that enables its use for self-regulating light activated control of fluid flow.
- Serena Seshadri
- , Luke F. Gockowski
- & Megan T. Valentine
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Article
| Open Access3D microstructure design of lithium-ion battery electrodes assisted by X-ray nano-computed tomography and modelling
The 3D microstructure of the electrode predominantly determines the electrochemical performance of Li-ion batteries. Here, the authors show that the microstructural heterogeneities lead to non-uniform Li insertion and current distribution while graded-microstructures improve the performance.
- Xuekun Lu
- , Antonio Bertei
- & Paul R. Shearing
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Article
| Open AccessPolyamide nanofiltration membrane with highly uniform sub-nanometre pores for sub-1 Å precision separation
Separating molecules or ions with sub-Angstrom scale precision is important but technically challenging. Here, the authors demonstrate that precise solute-solute separation can be achieved using polyamide membranes formed via surfactant-assembly regulated interfacial polymerization.
- Yuanzhe Liang
- , Yuzhang Zhu
- & Shihong Lin
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Article
| Open AccessCO oxidation activity of non-reducible oxide-supported mass-selected few-atom Pt single-clusters
Platinum nanocatalysts play critical roles in CO oxidation. Herein, the authors discover that under-coordinated Pt atoms at the edges of the first cluster layer are rendered cationic by direct contact with the Al2O3 support, which affects the overall CO oxidation activity.
- Atsushi Beniya
- , Shougo Higashi
- & Yoshihide Watanabe
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Article
| Open AccessReactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates
Reacting CO2 and ethane to achieve value-added C3 oxygenates offers opportunities to simultaneously reduce CO2 emissions and upgrade underutilized ethane in shale gas. Here, the authors report a successful oxygenate production strategy enabled by inserting CO2-derived CO into ethane-derived ethylene using a tandem reactor.
- Zhenhua Xie
- , Yuanguo Xu
- & Jingguang G. Chen
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Article
| Open AccessStrong metal-support interaction promoted scalable production of thermally stable single-atom catalysts
Large scale production of thermally stable single-atom catalysts (SACs) remains challenging. Here, the authors report scalable synthesis of Ru SACs by heating physical mixture of commercial RuO2 and Fe-containing support, which is significantly promoted by strong metal-support interaction.
- Kaipeng Liu
- , Xintian Zhao
- & Tao Zhang
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Article
| Open AccessHeterogeneous photoredox flow chemistry for the scalable organosynthesis of fine chemicals
Large-scale photochemical synthesis of high value chemicals is an ideal method of green chemical production. Here, the authors show the merging of heterogeneous carbon nitride photocatalysis with flow chemistry for the scalable organosynthesis of fine chemicals in a continuous flow reactor.
- Can Yang
- , Run Li
- & Xinchen Wang
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Article
| Open AccessPhoto splitting of bio-polyols and sugars to methanol and syngas
Methanol and syngas are important fuels and chemicals, which are presently produced from fossil resources. Here, the authors report the conversion of biomass-derived polyols and sugars into methanol and syngas via UV light irradiation under room temperature.
- Min Wang
- , Meijiang Liu
- & Feng Wang
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Article
| Open AccessSilica accelerates the selective hydrogenation of CO2 to methanol on cobalt catalysts
The hydrogenation of CO2 into valuable chemicals is greatly demanded, but suffers from complex product distribution. Here, the authors reported that, as a support and ligand, silica boosts cobalt catalysts to selectively hydrogenate CO2 into the desired methanol product.
- Lingxiang Wang
- , Erjia Guan
- & Feng-Shou Xiao
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Article
| Open AccessStable single platinum atoms trapped in sub-nanometer cavities in 12CaO·7Al2O3 for chemoselective hydrogenation of nitroarenes
Stabilize the active metal single atoms under harsh conditions is critical for the development of single atom catalysts. Here the authors report a nanoporous crystal, 12CaO·7Al2O3, that can firmly stabilize Pt single atoms in its surface cavities for efficient catalytic hydrogenation of nitroarenes.
- Tian-Nan Ye
- , Zewen Xiao
- & Hideo Hosono
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Article
| Open Access4D imaging of lithium-batteries using correlative neutron and X-ray tomography with a virtual unrolling technique
The combination of X-ray and neutron CT enables 4D studies, i.e. to explore the evolution of 3D structures with time. Here the authors apply this approach to a Li-ion primary cell, revealing elsewhere unseen trends in the spatial distribution of performance aided by a new ‘unrolling’ methodology.
- Ralf F. Ziesche
- , Tobias Arlt
- & Paul R. Shearing
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Article
| Open AccessSpatial quantification of dynamic inter and intra particle crystallographic heterogeneities within lithium ion electrodes
Dynamic chemical and structural heterogeneities within electrodes are known to lead to battery degradation and failure. Here, the authors show that X-ray diffraction computed tomography can be used to spatially quantify the dynamic crystallographic states of electrodes as they operate and degrade.
- Donal P. Finegan
- , Antonis Vamvakeros
- & Kandler Smith
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Article
| Open AccessLaminated self-standing covalent organic framework membrane with uniformly distributed subnanopores for ionic and molecular sieving
Fabrication of large scale and defect free covalent organic framework (COF) membranes with pores small enough for gas sieving remains challenging. Here, the authors report a scalable fabrication method to grow large area defect free COF membranes and to tune the pore size in the sub-nm region by adjusting the stacking modes of the COF layers.
- Yang Li
- , Qianxun Wu
- & Lijian Ma
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Article
| Open AccessRecover the activity of sintered supported catalysts by nitrogen-doped carbon atomization
Sintering supported metal nanoparticles is the common route to the deactivation of industrial heterogeneous catalysts. Here, the authors report a carbon atomization process that allows one not only to redisperse metal nanoparticles, but also to recover deactivated catalysts.
- Huang Zhou
- , Yafei Zhao
- & Yuen Wu
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Article
| Open AccessAcidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks
Increasing the strength of silanols in silica-aluminas can promote their catalytic activity in various applications. Here, the authors present a synergistic effect of two neighboring Al sites on the same silanol group, which can enhance the strength of silanol proton from moderate to zeolitic strength.
- Zichun Wang
- , Tong Li
- & Jun Huang
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Article
| Open AccessDouble layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold
Electrochemical CO2 reduction is a potential route to the sustainable production of valuable fuels and chemicals. In this joint experimental-theoretical work, the authors address the issue of the rate-limiting step on Gold and present insights from multi-scale simulations into the importance of the electric double layer on reaction kinetics and mass transport.
- Stefan Ringe
- , Carlos G. Morales-Guio
- & Karen Chan
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Article
| Open AccessInterfacial Fe5C2-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols
Long-chain alcohols synthesis from syngas conversion is a promising route for the production of high-value chemicals. Here the authors show that a heterogeneous Fe5C2/Cu catalyst derived from layered double hydroxides precursor exhibits excellent performance with a space time yield of 0.101 g gcat−1 h−1 at a low pressure of 1 MPa.
- Yinwen Li
- , Wa Gao
- & Ding Ma
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Review Article
| Open AccessDesign principles of ion selective nanostructured membranes for the extraction of lithium ions
Lithium is in increasing demand for energy storage and is abundant in seawater, but its extraction is challenging due to coexistence with similar ions. Here the authors review recent advances in lithium separation strategies, focusing on the development of nanochannel and nanopore based membranes.
- Amir Razmjou
- , Mohsen Asadnia
- & Vicki Chen
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Perspective
| Open AccessCO2 hydrogenation to high-value products via heterogeneous catalysis
Carbon dioxide (CO2) capture and conversion provide an alternative approach to synthesis of useful fuels and chemicals. Here, Ye et al. give a comprehensive perspective on the current state of the art and outlook of CO2 catalytic hydrogenation to the synthesis of light olefins, dimethyl ether, liquid fuels, and alcohols.
- Run-Ping Ye
- , Jie Ding
- & Yuan-Gen Yao
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Article
| Open AccessPalladium-bearing intermetallic electride as an efficient and stable catalyst for Suzuki cross-coupling reactions
In Suzuki coupling reactions, excellent catalytic performance require negatively charged Pd species and the avoidance of metal leaching or clustering. Here the authors implanted Pd sites into an intermetallic electride, Y3Pd2, which serves as an efficient and stable catalyst for Suzuki coupling reactions.
- Tian-Nan Ye
- , Yangfan Lu
- & Hideo Hosono
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Article
| Open AccessNear 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation
Chemical looping methane partial oxidation is an effective technology to produce syngas with a minimal energy penalty. Here, the authors design and develop a mesoporous silica supported nanoparticle oxygen carrier that enables a near 100% CO generation with high recyclability and substantially lower operating temperature.
- Yan Liu
- , Lang Qin
- & Liang-Shih Fan
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Article
| Open Access3D designed and printed chemical generators for on demand reagent synthesis
Synthetic labs rely on a vast number of chemicals, which are often unstable with time and affected by price fluctuations. Here, the authors report ad hoc developed cartridge reactionware for the synthesis of four different targets in a time- and cost-saving manner.
- Sergey S. Zalesskiy
- , Philip J. Kitson
- & Leroy Cronin
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Article
| Open AccessStructural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides
The authors here look into the phase transitions in Li-/Mn-rich layered cathode materials during synthesis and cycling. It is revealed that the Li-rich layered structure tends to transform to a Li-poor spinel phase via an intermediate Li-containing rock salt phase, with release of lithium/oxygen.
- Weibo Hua
- , Suning Wang
- & Björn Schwarz
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Article
| Open AccessGeneral technoeconomic analysis for electrochemical coproduction coupling carbon dioxide reduction with organic oxidation
Coupling of carbon dioxide reduction and organic oxidation is promising for sustainable chemicals production; however, economics are impacted by variations in product combinations and process design. Here the authors report technoeconomic analysis for a range of technologies and coproduction processes.
- Jonggeol Na
- , Bora Seo
- & Ung Lee
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Article
| Open AccessCatalytic production of impurity-free V3.5+ electrolyte for vanadium redox flow batteries
The vanadium redox flow battery is promising for commercial applications, but is hampered by high-cost electrolytes that are typically prepared via electrolysis. Here the authors demonstrate cost-effective chemical production of a high-quality vanadium electrolyte using platinum nanoparticles as a catalyst.
- Jiyun Heo
- , Jae-Yun Han
- & Hee-Tak Kim
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Article
| Open AccessMaximizing sinusoidal channels of HZSM-5 for high shape-selectivity to p-xylene
Full utilization of ZSM-5 shape-selectivity is restricted by crystal external surface acid sites and co-existence of two different sized channels. Here, the authors synthesize reverse Al zoned ZSM-5 with sinusoidal channel preferentially opened to its inert external surface to achieve 99.3% p-xylene selectivity.
- Chuanfu Wang
- , Lei Zhang
- & Ding Ma
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Article
| Open AccessA chemo-enzymatic oxidation cascade to activate C–H bonds with in situ generated H2O2
Continuous low-level supply or in situ generation of hydrogen peroxide (H2O2) is essential for the stability of unspecific peroxygenases. Here, the authors demonstrate that AuPd / TiO2 can generate sufficient H2O2 for the engineered unspecific heme-thiolate peroxygenase PaDa-I to oxidise a range of C-H bonds.
- Simon J. Freakley
- , Svenja Kochius
- & Graham J. Hutchings
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Article
| Open AccessDesign and synthesis of highly active MoVTeNb-oxides for ethane oxidative dehydrogenation
Crystalline M1 phase of Mo-V-Te-Nb mixed oxide is an excellent catalyst for ethane oxidative dehydrogenation to ethene. Here, the authors show a method that synthesizes highly active materials by generating M1 crystals with corrugated terminations, thus exposing a large concentration of active sites.
- Daniel Melzer
- , Gerhard Mestl
- & Johannes A. Lercher
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Article
| Open AccessSurpassing the single-atom catalytic activity limit through paired Pt-O-Pt ensemble built from isolated Pt1 atoms
Single-atom metal catalysts offer maximized material efficiency, but there is large room to improve the intrinsic activity per metal atom for many reactions. Here, the authors demonstrate that the solution for CO oxidation is to tackle the issue of lacking neighboring Pt atoms in the single-atom Pt1/CeO2 system.
- Hui Wang
- , Jin-Xun Liu
- & Ming Yang
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Article
| Open AccessIsolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles to regulate selectivity in 4-nitrophenylacetylene hydrogenation
Noble metals play a momentous role in heterogeneous catalysis but still face a huge challenge in selectivity control. Herein, the authors demonstrate that isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles is an effective strategy to optimize the selectivity of Pt catalysts.
- Aijuan Han
- , Jian Zhang
- & Yadong Li
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Article
| Open AccessTuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
Converting solar energy to hydrogen fuel requires light-absorbers that well-match the wavelengths of incoming sunlight. Here, authors prepare a broadband visible-light-absorbing molecular complex that efficiently produces hydrogen from water.
- Ji Hoon Lee
- , Shyam Kattel
- & Jingguang G. Chen
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Article
| Open AccessA versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
The general synthesis of single atom catalysts (SACs) is of broad interest to chemists but remains a formidable challenge. Here, with the precursor-dilution strategy, the authors successfully prepare 24 different SACs and the Pt SACs exhibit superior chemo- and regio-selectivity in hydrogenation.
- Xiaohui He
- , Qian He
- & Hongbing Ji
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Article
| Open AccessBand-collision gel electrophoresis
Electrophoretic mobility shift assays are widely used in gel electrophoresis to study binding interactions between different molecular species, but these assays access only a subset of reaction possibilities. Here, the authors develop a band-collision gel electrophoresis (BCGE) approach that demonstrates a much wider variety of reaction types.
- Dimitri A. Bikos
- & Thomas G. Mason
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Article
| Open AccessAtomic
- scale engineering of indium oxide promotion by palladium for methanol production via CO2 hydrogenationGenerating and quantifying the effect of the promoter speciation in heterogeneous catalysts is very challenging. Here, the authors show that the precise palladium atoms architecture reached by controlled co-precipitation overcomes selectivity and stability limitations associated with palladium nanoparticles for CO2-based methanol synthesis.
- Matthias S. Frei
- , Cecilia Mondelli
- & Javier Pérez-Ramírez
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Article
| Open AccessTrade-off in membrane distillation with monolithic omniphobic membranes
Omniphobic membranes are attractive for membrane distillation because of their superior wetting resistance. Here the authors develop a particle-free approach for rapid fabrication of monolithic omniphobic membranes and elucidate the underlying mechanism of wetting resistance-vapor permeability trade-off in membrane distillation desalination.
- Wei Wang
- , Xuewei Du
- & Tiezheng Tong
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Review Article
| Open AccessFundamentals and applications of photocatalytic CO2 methanation
While natural gas and fossil fuels power human activities, increasing concerns over fuel reserves and environmental impacts require finding alternative, renewable resources. Here, authors review the fundamental science and progress on solar-powered conversion of carbon dioxide to methane.
- Ulrich Ulmer
- , Thomas Dingle
- & Geoffrey A. Ozin
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Article
| Open AccessThermoresponsive nanoemulsion-based gel synthesized through a low-energy process
Hydrogel emulsions enable facile loading of bioactive compounds but fabrication methods which allow upscaling and low cytotoxicity are scarce. Here, the authors report a thermally triggered low energy gelation mechanism based on the interaction between a nontoxic Pluronic and nanoemulsion droplets.
- Seyed Meysam Hashemnejad
- , Abu Zayed Md Badruddoza
- & Patrick S. Doyle
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Article
| Open AccessAn ultrathin conformable vibration-responsive electronic skin for quantitative vocal recognition
Though skin-attachable vibration sensors are promising for voice recognition applications, current technologies do not meet key performance requirements. Here, the authors report a flexible skin-attachable sensor with high sensitivity and flat frequency response over the vocal frequency range.
- Siyoung Lee
- , Junsoo Kim
- & Kilwon Cho
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Article
| Open AccessInkjet-printed stretchable and low voltage synaptic transistor array
The development of novel low-cost fabrication schemes for realizing stretchable transistor arrays with applicability in wearable electronics remains a challenge. Here, the authors report skin-like electronics with stretchable active materials and devices processed exclusively from ink-jet printing.
- F. Molina-Lopez
- , T. Z. Gao
- & Z. Bao
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Article
| Open AccessTuning the permselectivity of polymeric desalination membranes via control of polymer crystallite size
Increasing the selectivity of desalination membranes is of crucial importance for advancing membrane desalination technologies. Here the authors demonstrate a plasticizing-extracting process for tuning the permselectivity of polymeric membranes and achieving desired desalination performance.
- Xinglin Lu
- , Xunda Feng
- & Menachem Elimelech
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Article
| Open AccessTuning porosity in macroscopic monolithic metal-organic frameworks for exceptional natural gas storage
While metal–organic frameworks exhibit record-breaking gas storage capacities, their typically powdered form hinders their industrial applicability. Here, the authors engineer UiO-66 into centimetre-sized monoliths with optimal pore-size distributions, achieving benchmark volumetric working capacities for both CH4 and CO2.
- B. M. Connolly
- , M. Aragones-Anglada
- & D. Fairen-Jimenez
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Article
| Open AccessEffect of molecular architecture on ring polymer dynamics in semidilute linear polymer solutions
Understanding the dynamics of ring polymers is challenging are despite recent progress, understanding of the nonequilibrium behavior of ring polymers has not yet been achieved. Here, the authors directly observe the flow dynamics of DNA-based rings in semidilute linear polymer solutions using single molecule techniques.
- Yuecheng Zhou
- , Kai-Wen Hsiao
- & Charles M. Schroeder
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Article
| Open AccessDesign of next-generation ceramic fuel cells and real-time characterization with synchrotron X-ray diffraction computed tomography
Miniaturized ceramic fuel cells are attractive for portable devices, but performance should be optimized. Here the authors report a micro-monolithic ceramic cell design for a tubular solid oxide fuel cell containing a multi-channel anode support with enhanced power density and stable operation.
- Tao Li
- , Thomas M. M. Heenan
- & Kang Li
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Article
| Open AccessCritical role of formaldehyde during methanol conversion to hydrocarbons
The recognition of the importance of HCHO in methanol to olefins (MTO) makes it imperative to quantify its concentration in the reaction and distribution over the catalyst bed. Here the authors quantify the concentration level of HCHO and its distribution along the catalyst bed in MTO, and explores its role in methanol conversion.
- Yue Liu
- , Felix M. Kirchberger
- & Johannes A. Lercher
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Article
| Open AccessFabrication of arbitrary three-dimensional suspended hollow microstructures in transparent fused silica glass
Fused silica glass has excellent optical properties, chemical and thermal stability and hardness, but its microstructuring for miniaturized applications has proven difficult. Here the authors demonstrate obtainment of precise arbitrary three dimensional hollow microstructures in fused silica glass by sacrificial template replication.
- Frederik Kotz
- , Patrick Risch
- & Bastian E. Rapp
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Article
| Open AccessDirect conversion of CO and H2O into liquid fuels under mild conditions
Developing new carbon resource transformation protocols leading to the production of liquid fuels with high selectivity under mild conditions remains challenging. Here the authors present a novel and energy-efficient catalytic route to directly transform CO and H2O to liquid fuels at low temperature in aqueous phase.
- Yao Xu
- , Jing Li
- & Ding Ma