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| Open AccessVisualizing the multi-level assembly structures of conjugated molecular systems with chain-length dependent behavior
A deep understanding of multi-level assembly structures of conjugated polymers is crucial for developing high performance conjugated polymers and optoelectronic devices, however, it remains a challenge. Here, the authors report the morphological evolution of multi-level assembly of a model system of isoindigo-based conjugated polymer.
- Yang-Yang Zhou
- , Yu-Chun Xu
- & Jian Pei
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Article
| Open AccessAcetolysis of waste polyethylene terephthalate for upcycling and life-cycle assessment study
The recycling of polyethylene terephthalate is of utmost importance to reduce environmental pollution and reliance on fossil resources however, the existing methods do not process colored or blended polyethylene terephthalate materials. Here, the authors demonstrate the acetolysis of waste polyethylene terephthalate into terephthalic acid and simultaneous acidic degradation of dyes and additives
- Yuantao Peng
- , Jie Yang
- & Yao Fu
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Article
| Open AccessA strong bimetal-support interaction in ethanol steam reforming
Ethanol steam reforming (ESR) reaction is an environmentally benign and sustainable route for H2 production. Herein, the authors demonstrate a conceptional strategy for rational design and preparation of highly-efficient catalyst toward ESR via an RhNi-TiO2 strong bimetal-support interaction.
- Hao Meng
- , Yusen Yang
- & Xue Duan
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Article
| Open AccessDual-site catalysts featuring platinum-group-metal atoms on copper shapes boost hydrocarbon formations in electrocatalytic CO2 reduction
The inclusion of platinum-group metals for CO2 reduction electrocatalyst design may trigger the unwanted hydrogen evolution reaction. However, here the authors show that single-atom Pd and Pt on facet-selective Cu can selectively boost CO2 to CH4 or C2H4 conversion through dual-site pathways.
- Manjeet Chhetri
- , Mingyu Wan
- & Ming Yang
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Article
| Open AccessFrictional fluid instabilities shaped by viscous forces
Fingering patterns form spontaneously when a non-wetting viscous liquid displaces a dry granular mixture in a confined flow cell. The authors show how these patterns are controlled by the balance between viscous, capillary, and frictional forces.
- Dawang Zhang
- , James M. Campbell
- & Bjørnar Sandnes
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Article
| Open AccessSelective formation of acetate intermediate prolongs robust ethylene removal at 0 °C for 15 days
Efficient ethylene removal below room temperatures is of great importance to food transportation and storage. Here the authors have developed an efficient gold-platinum nanoalloy catalyst for trace ethylene removal at 0 °C for 15 days.
- Mingyue Lin
- , Haifeng Wang
- & Toru Murayama
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Article
| Open AccessApproaching enzymatic catalysis with zeolites or how to select one reaction mechanism competing with others
Approaching the level of molecular recognition of enzymes with solid catalysts is a challenging goal. Here, the authors present a computational methodology that guides the selection of the most adequate zeolite frameworks for target reactions.
- Pau Ferri
- , Chengeng Li
- & Avelino Corma
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Article
| Open AccessAqueous phase conversion of CO2 into acetic acid over thermally transformed MIL-88B catalyst
Carbon dioxide conversion into chemicals is essential for carbon capture and utilization. Here, the authors present a novel iron-based catalyst, synthesized from the thermal treatment of a parent metal-organic framework (MIL-88B), to produce a dual-active site for carbon dioxide reduction into acetic acid.
- Waqar Ahmad
- , Paramita Koley
- & Akshat Tanksale
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Article
| Open AccessUpscaled production of an ultramicroporous anion-exchange membrane enables long-term operation in electrochemical energy devices
The design of highly selective yet robust anion exchange membranes remains a challenge. Here, the authors prepare a stable polymer membrane composed of terphenyl isomers, demonstrate roll-to-roll manufacturing, and assess its properties in redox flow batteries, water electrolyzers and fuel cells.
- Wanjie Song
- , Kang Peng
- & Tongwen Xu
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Article
| Open AccessMemory-dictated dynamics of single-atom Pt on CeO2 for CO oxidation
The use of single atoms of platinum group metals on CeO2 is a promising approach to reduce precious metal requirements for automobile exhaust treatment catalysts. Here, the authors discovered that by manipulating the calcination temperatures, they could control the configuration of Pt1 on the CeO2 surface, leading to differences in CO oxidation activity.
- Zihao Zhang
- , Jinshu Tian
- & Yong Wang
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Article
| Open AccessSurface manipulation for prevention of migratory viscous crude oil fouling in superhydrophilic membranes
Minimizing membrane fouling is critical for their continuous and efficient operation. Here, authors demonstrate a wrinkled-pattern microparticles-decorated membrane surface can increase contact area with water molecules, expand steric hindrance, and inhibit adhesion and deposition of oil, achieving efficient migratory viscous crude oil antifouling.
- Yuanyuan Zhao
- , Xiaobin Yang
- & Lu Shao
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Article
| Open Access4D nanoimaging of early age cement hydration
In this work, the authors use near-field ptychographic nanotomography to visualize cement hydration in situ. They report hydration features with submicrometer detail including calcium silicate dissolution rates, etch-pit growth rates and water-to-air porosity evolution.
- Shiva Shirani
- , Ana Cuesta
- & Miguel A. G. Aranda
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Article
| Open AccessSelective conversion of CO2 to isobutane-enriched C4 alkanes over InZrOx-Beta composite catalyst
Direct conversion of CO2 to a specific hydrocarbon with high selectivity is attractive but challenging. Here the authors report a highly active InZrOx-Beta tandem catalyst for CO2 hydrogenation to butane and develop a surface silica protection strategy to inhibit the migration of indium species, greatly improving catalytic stability.
- Han Wang
- , Sheng Fan
- & Jianguo Wang
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Article
| Open AccessStructure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation
Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation but suffer from instability and difficulty in catalyst recycling. Here the authors design an atomically dispersed Ir catalyst which can be considered the bridge between homogeneous and heterogeneous catalysis and displays an outstanding catalytic performance in n-butane dehydrogenation.
- Xiaowen Chen
- , Xuetao Qin
- & Ding Ma
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Article
| Open AccessConcerted oxygen diffusion across heterogeneous oxide interfaces for intensified propane dehydrogenation
Non-oxidative dehydrogenation technologies suffer from the thermodynamic equilibrium limitations and severe coking. Here, the authors report the intensified propane dehydrogenation to propylene by the chemical looping engineering on nanoscale core-shell redox catalysts.
- Sai Chen
- , Ran Luo
- & Jinlong Gong
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Article
| Open AccessRhodium nanoparticles supported on silanol-rich zeolites beyond the homogeneous Wilkinson’s catalyst for hydroformylation of olefins
Heterogeneous catalysts for olefin hydroformylation are highly desired but suffer from poor activity. Herein, the authors report that rhodium nanoparticles supported on siliceous MFI zeolite with abundant silanol nests are very active for hydroformylation, affording a turnover frequency that outperforms the classical Wilkinson’s catalyst.
- Yifeng Liu
- , Zhiqiang Liu
- & Feng-Shou Xiao
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Article
| Open AccessElectrosynthesis of chlorine from seawater-like solution through single-atom catalysts
Chlor-alkali process plays an important role in the chemical industry. However, large overpotential and low selectivity of currently used catalysts lead to high energy consumption. Here the authors report Ru-O4 single site catalysts for chlorination evolution with 1000 h stability at 1000 mA cm−2 in a seawater-like environment.
- Yangyang Liu
- , Can Li
- & Shenlong Zhao
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Article
| Open AccessPhotothermal-enabled single-atom catalysts for high-efficiency hydrogen peroxide photosynthesis from natural seawater
Photoproduction of solar fuels and important chemicals is of significant interest. Here, the authors construct a cobalt single atom-based photothermal-photocatalytic heterostructure that realizes efficient hydrogen peroxide photosynthesis from earth-abundant seawater.
- Wei Wang
- , Qun Song
- & Ning Wang
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Article
| Open AccessAchieving volatile potassium promoted ammonia synthesis via mechanochemistry
Potassium oxide is used as a promotor in industrial ammonia synthesis, although metallic potassium is better in theory. Here, the authors demonstrate metallic potassium, an unstable metal that easily volatilizes at high temperature, can be used as a promotor for ammonia synthesis.
- Jong-Hoon Kim
- , Tian-Yi Dai
- & Jong-Beom Baek
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Article
| Open AccessPyro-layered heterostructured nanosheet membrane for hydrogen separation
Engineering 2D heterostructures with unique physiochemical properties and molecular sieving channels is one approach for designing membranes selective gas molecule transport. Here authors arrange graphene and boron nitride nanosheets in an alternating pattern, resulting in narrow porous nanochannels and excellent hydrogen separation properties.
- Ruoxin Wang
- , Jianhao Qian
- & Huanting Wang
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Article
| Open AccessCoupling acid catalysis and selective oxidation over MoO3-Fe2O3 for chemical looping oxidative dehydrogenation of propane
A MoO3-Fe2O3 redox catalyst with dispersed Mo species on γ-Fe2O3 is synthesized for the oxidative dehydrogenation of propane via chemical looping. Acid sites and lattice oxygen regulation promote the production of and selectivity for propylene.
- Xianhui Wang
- , Chunlei Pei
- & Jinlong Gong
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Article
| Open AccessBr−/BrO−-mediated highly efficient photoelectrochemical epoxidation of alkenes on α-Fe2O3
Alkene epoxidation, whose products are important intermediates for the manufacture of pharmaceuticals and epoxy resins, has attracted extensive attention. Unlike the conventional electrochemical Br−/Br2-mediated epoxidation, here the authors report a photoelectrochemical Br−/BrO−- mediated system to achieve efficient epoxidation performance on α-Fe2O3.
- Yukun Zhao
- , Mengyu Duan
- & Jincai Zhao
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Article
| Open AccessDirect synthesis of extra-heavy olefins from carbon monoxide and water
Fischer-Tropsch synthesis is challenged by the trade-off between enhancing C-C coupling and suppressing further hydrogenation of olefins. Here the authors break this challenge by developing a universal strategy to synthesis extra-heavy olefins from carbon monoxide and water via the sustained release of hydrogen and selective extraction of olefins.
- Chuanhao Wang
- , Junjie Du
- & Jie Zeng
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Article
| Open AccessBoosting membrane carbon capture via multifaceted polyphenol-mediated soldering
The development of mixed-matrix membranes is especially challenging when highly permeable materials are used. Here the authors present a molecular soldering strategy featuring multifunctional polyphenols in tailored polymer chains, well-designed hollow MOF structures, and defect-free interfaces to break the permeability-selectivity trade-off limit.
- Bin Zhu
- , Shanshan He
- & Lu Shao
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Article
| Open AccessEquilibrium shift, poisoning prevention, and selectivity enhancement in catalysis via dehydration of polymeric membranes
Generation of water as a byproduct in chemical reactions is often detrimental because it lowers the yield of the target product. Here, a thermally rearranged polybenzoxazole membrane has been developed, allowing for selective removal of water in chemical reactions.
- Myeong-Hun Hyeon
- , Hae-Gu Park
- & Seok Ki Kim
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Article
| Open AccessContinuous ammonia electrosynthesis using physically interlocked bipolar membrane at 1000 mA cm−2
Achieving stable and continuous NH3 electrosynthesis is of great interests. Here, the authors report a bipolar membrane with a three-dimensional physically interlocked interface to achieve a continuous NH3 production from nitrate electroreduction at 1000 mA cm−2 for over 100 h.
- Ziang Xu
- , Lei Wan
- & Baoguo Wang
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Article
| Open AccessHigh production of furfural by flash pyrolysis of C6 sugars and lignocellulose by Pd-PdO/ZnSO4 catalyst
Furfural is an important platform chemical for the synthesis of next-generation bio-fuels. Here the authors report a novel heterogeneous catalyst, Pd-PdO/ZnSO4, for the mass production of furfural from catalytic flash pyrolysis of lignocellulosic biomasses.
- Qiaoqiao Zhou
- , Jinxing Gu
- & Lian Zhang
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Article
| Open AccessAlphaFlow: autonomous discovery and optimization of multi-step chemistry using a self-driven fluidic lab guided by reinforcement learning
Autonomous exploration of materials design space is hindered by its high dimensionality and the scarcity of data. In this work, we present AlphaFlow, a self-driven lab guided by reinforcement learning that enables accelerated discovery and optimization of multi-step chemistries.
- Amanda A. Volk
- , Robert W. Epps
- & Milad Abolhasani
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Article
| Open AccessUltrahigh loading dry-process for solvent-free lithium-ion battery electrode fabrication
Scalable dry electrode process is essential for the sustainable manufacturing of the lithium based batteries. Here, the authors propose a dry press-coating technique to fabricate a robust and flexible high loading electrode for lithium pouch cells.
- Minje Ryu
- , Young-Kuk Hong
- & Jong Hyeok Park
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Article
| Open AccessEx-situ generation and synthetic utilization of bare trifluoromethyl anion in flow via rapid biphasic mixing
The trifluoromethyl anion rapidly decomposes into difluorocarbene (:CF2) and fluorine ion, limiting its applicability in synthesis. Here, the authors report a strategy to generate and use the short-lived CF3- intermediate from stable CF3H gas via fast biphasic mixing in precisely customized flow dissolvers.
- Hyune-Jea Lee
- , Jeong-Un Joo
- & Heejin Kim
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Article
| Open AccessProbing sub-5 Ångstrom micropores in carbon for precise light olefin/paraffin separation
Achieving highly selective separation of olefin/paraffin is a significant challenge in the chemical industry. Here the authors present polydopamine-derived carbons with tailorable sub-5 Å micropores probed by a series of gas molecules that can realize precise size-sieving of olefin from paraffin.
- Shengjun Du
- , Jiawu Huang
- & Banglin Chen
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Article
| Open AccessScalable synthesis of Cu clusters for remarkable selectivity control of intermediates in consecutive hydrogenation
Scalable synthesis of stable Cu clusters for heterogeneous catalysis is still a major challenge. Here the authors report a low-temperature atomic diffusion approach for synthesis of stable Cu cluster catalysts, which exhibit high yield of intermediate product in consecutive hydrogenation reactions.
- Dawei Yao
- , Yue Wang
- & Xinbin Ma
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Article
| Open AccessPolyamide membranes with nanoscale ordered structures for fast permeation and highly selective ion-ion separation
Membranes with precise ion-ion separation are critical for sustainable water treatment. Here, authors demonstrated controlled construction of a nanofiltration membrane with fast permeation and high Cl-/SO42- selectivity by simultaneous spatial and temporal control of interfacial polymerization.
- Changwei Zhao
- , Yanjun Zhang
- & Sui Zhang
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Article
| Open AccessDeformation constraints of graphene oxide nanochannels under reverse osmosis
Nanochannels in laminated graphene oxide nanosheets featuring confined mass transport have attracted interest in multiple research fields. As an important aspect for efficient pressure-driven membrane processes, authors investigate the response and deformation behaviours of such nanochannels to different external conditions.
- Kecheng Guan
- , Yanan Guo
- & Hideto Matsuyama
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Article
| Open AccessLife cycle net energy assessment of sustainable H2 production and hydrogenation of chemicals in a coupled photoelectrochemical device
Integrating green hydrogen production with the generation of valuable chemicals has the potential to increase the competitiveness of the system. Here, the authors quantitatively evaluate the energetic benefit of coupling hydrogen production with the hydrogenation of feedstocks in a photoelectrochemical device.
- Xinyi Zhang
- , Michael Schwarze
- & Fatwa F. Abdi
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Article
| Open AccessLong-lifetime water-washable ceramic catalyst filter for air purification
Disposable filters are generally used for air purification despite frequent replacement and waste generation problems. Here, a ceramic catalyst filter is introduced as a new class of filter that simultaneously removes PMs and VOCs as primary air pollutants and can be regenerated and used for long periods by simple water washing.
- Hyuk Jae Kwon
- , Dong Sik Yang
- & Hyun Chul Lee
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Article
| Open AccessPhotocatalytic cyclohexane oxidation and epoxidation using hedgehog particles
Spiky hedgehog particles are reported to access a photocatalytic pathway for alkane oxidation directly to industrially relevant epoxides in one step, providing a lower cost and less energy-intensive pathway as compared to common alkene feedstocks.
- Douglas G. Montjoy
- , Elizabeth A. K. Wilson
- & Nicholas A. Kotov
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Article
| Open AccessEngineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx
Boosting activity of oxide catalysts is a long-lasting challenge to developing efficient catalysts for industrially important reactions such as CO2-to-methanol. Here, the authors report a strategy for enhancing the activity of a ZnZrOx methanol synthesis catalyst via engineered nanoscale H supply.
- Kyungho Lee
- , Paulo C. D. Mendes
- & Ning Yan
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Article
| Open AccessMalodour classification with low-cost flexible electronics
Designing machine learning hardware on flexible substrates is promising for several applications. Here, the authors propose an integrated smart system built with low-cost flexible electronics components for classifying human malodour, and demonstrates that the proposed system scores malodour as good as expert human assessors.
- Emre Ozer
- , Jedrzej Kufel
- & Jane Ford
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Article
| Open AccessDirect synthesis of ordered mesoporous materials from thermoplastic elastomers
Scaled manufacturing of ordered mesoporous materials has been historically challenging. This work reports a simple and generalizable method to directly convert low-cost thermoplastic elastomers to mesoporous polymer, carbon, and silica, with controlled pore textures by altering precursor identity.
- Mark Robertson
- , Alejandro Guillen-Obando
- & Zhe Qiang
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Article
| 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