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| Open AccessFrustrated Lewis pair catalyst realizes efficient green diesel production
The commercial production of green diesel suffers from the requirement for continuous sulfur replenishment to maintain catalytic activity. Here, the authors report a sulfur-free catalytic system that can efficiently produce green diesel from various feedstocks over long periods of operation.
- De-Chang Li
- , Zhengyi Pan
- & Guang-Hui Wang
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Article
| Open AccessLow-nuclearity CuZn ensembles on ZnZrOx catalyze methanol synthesis from CO2
The ideal metal selection and atomic-level arrangement for catalysts in CO2 hydrogenation are still uncertain. Here, copper is identified as the most effective promoter for enhancing ZnZrOx catalysts when precisely structured into CuZn ensembles, offering new insights for designing superior catalysts for CO2-based methanol synthesis.
- Thaylan Pinheiro Araújo
- , Georgios Giannakakis
- & Javier Pérez-Ramírez
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Article
| Open AccessPd/NiMoO4/NF electrocatalysts for the efficient and ultra-stable synthesis and electrolyte-assisted extraction of glycolate
Here, the authors report a path for electrocatalytic conversions of alcohols through in-situ acid-base reaction and the design of electrocatalysts. In this work, the electrocatalyst had reduced Pd content, improved efficiency, and lowered costs.
- Kai Shi
- , Di Si
- & Jianlin Shi
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Article
| Open AccessExtreme Li-Mg selectivity via precise ion size differentiation of polyamide membrane
Achieving high selectivity of Li+ and Mg2+ is of paramount importance for effective lithium extraction from brines, and nanofiltration (NF) membrane plays a critical role in this process. Here the authors report the fabrication of polyamide NF membranes with ultra-high Li + /Mg2+ selectivity by modifying the interfacial polymerization process with an oil-soluble surfactant.
- Quan Peng
- , Ruoyu Wang
- & Lei Jiang
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Article
| Open AccessBiobased and biodegradable films exhibiting circularly polarized room temperature phosphorescence
Sustainable materials with circularly polarized room-temperature phosphorescence are desirable but challenging to design. Here, the authors report the development of thin films, based on cellulose nanocrystals and lignosulfonate, with circularly polarised room temperature phosphorescence.
- Mengnan Cao
- , Yiran Ren
- & Zhijun Chen
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Article
| Open AccessSelective hydrodeoxygenation of α, β-unsaturated carbonyl compounds to alkenes
The selective reduction of α, β-unsaturated carbonyls remains a challenge. Here the authors report a zinc-based catalyst for this reaction, converting α, β-unsaturated carbonyl compounds into unsaturated alcohols followed by hydrodeoxygenation to form alkenes.
- Tianjiao Wang
- , Yu Xin
- & Buxing Han
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Article
| Open AccessUltrathin, ultralight dual-scale fibrous networks with high-infrared transmittance for high-performance, comfortable and sustainable PM0.3 filter
Development of high-performance, comfortable and sustainable air filters is challenging. Here, authors design an ultrathin, ultralight dual scale fiber mat composed of true nanofibers and submicron-fibers to integrate the high protection, thermal wet comfort and save raw materials.
- Yuchen Yang
- , Xiangshun Li
- & Yuekun Lai
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Article
| Open AccessEfficient catalyst-free N2 fixation by water radical cations under ambient conditions
The growth and sustainable development of humanity is heavily dependent upon N2 fixation. Herein, authors developed an ambient catalyst-free disproportionation of N2 by water plasma to yield economically valuable nitroxyl and hydroxylamine products.
- Xiaoping Zhang
- , Rui Su
- & Huanwen Chen
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Article
| Open AccessComputational redesign of a hydrolase for nearly complete PET depolymerization at industrially relevant high-solids loading
The application of the LCC variant of polyethylene terephthalate (PET) hydrolase for industrial degradation of PET has been hindered by the 10% of nonbiodegradable PET. Here, the authors use a computational strategy to engineer TurboPETase which outperforms other PETase variants and achieves nearly complete depolymerization of the postconsumer PET bottles at a high, industrially relevant, level of solids loading.
- Yinglu Cui
- , Yanchun Chen
- & Bian Wu
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Article
| Open AccessDecoupled electrolysis for hydrogen production and hydrazine oxidation via high-capacity and stable pre-protonated vanadium hexacyanoferrate
Decoupled electrolysis with the aid of a redox mediator offers great flexibility in operation. Here, the authors construct a decoupled electrolysis system for separate hydrogen production and electricity generation to achieve flexible energy conversion and storage using renewables.
- Fei Lv
- , Jiazhe Wu
- & Yubin Chen
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Article
| Open AccessMediating trade-off between activity and selectivity in alkynes semi-hydrogenation via a hydrophilic polar layer
The semi-hydrogenation of alkynes faces the trade-off between activity and selectivity due to undesirable over-hydrogenation. Here the authors report an efficient additive-free WO3-based single-atom Pd catalytic system with a vertical size effect of hydrogen spillover to mediate the trade-off between activity and selectivity.
- Jinqi Xiong
- , Shanjun Mao
- & Yong Wang
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Article
| Open AccessOne-pot redox cascade paired electrosynthesis of gamma-butyrolactone from furoic acid
Paired electrolysis is challenging without membrane and redox mediators. The authors developed a one-pot, mediator-free, and scalable e-synthesis of γ-butyrolactone (GBL) from furoic acid with high yield and selectivity in an aqueous electrolyte.
- Shengqin Liu
- , Yangxin Jin
- & Jason Chun-Ho Lam
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Article
| Open AccessPhoto-thermal coupling to enhance CO2 hydrogenation toward CH4 over Ru/MnO/Mn3O4
Reduction of CO2 with solar energy is an attractive route to new fuel sources. Here a nanostructured Ru/MnOx photo-thermal catalyst composed of well-defined Ru/MnO/Mn3O4 is reported for CO2 hydrogenation with high selectivity and a CH4 production rate at a mild temperature of 200 °C.
- Jianxin Zhai
- , Zhanghui Xia
- & Buxing Han
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Article
| Open AccessMechanochemical synthesis of organoselenium compounds
While the reported methods for the synthesis of organoselenium compounds mainly employ preformed activated selenium reagents, the direct utilization of elemental selenium in the synthesis is a more attractive but challenging strategy. Here, the authors report the rapid synthesis of versatile organoselenium compounds via mechanical stimulation.
- Shanshan Chen
- , Chunying Fan
- & Xiaofeng Wei
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Article
| Open AccessAqueous amine enables sustainable monosaccharide, monophenol, and pyridine base coproduction in lignocellulosic biorefineries
Utilization of the entire lignocellulose is essential for sustainable and cost-effective biorefineries, but it is hindered by a trade-off between efficient carbohydrate utilization and lignin-to-chemical conversion yield. Here, the authors report a mild lignocellulosic fractionation process using aqueous diethylamine which produces a carbohydrate fraction susceptible to enzymatic hydrolysis and a high-quality lignin that delivers high monomer yields upon catalytic amination and depolymerization.
- Li Xu
- , Meifang Cao
- & Xueqing Qiu
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Article
| Open AccessUnlocking osmotic energy harvesting potential in challenging real-world hypersaline environments through vermiculite-based hetero-nanochannels
Harvesting osmotic energy in real world high-salinity solutions poses great challenges, authors propose nanofluidic membranes with a dual separation mechanism based on vermiculite nanosheets with an isomorphic substitution structure, showing excellent energy conversion in hypersaline environments.
- Jin Wang
- , Zheng Cui
- & Lei Wang
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Article
| Open AccessSolar-driven membrane separation for direct lithium extraction from artificial salt-lake brine
An efficient and cost-effective Mg/Li separation process is necessary for lithium extraction from Salt Lake brines. Inspired by the mangroves, authors developed a direct lithium extraction method from Salt Lake brines through the synergistic effect of an ion separation membrane and a solar evaporator.
- Shenxiang Zhang
- , Xian Wei
- & Jian Jin
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Article
| Open AccessA general strategy for recycling polyester wastes into carboxylic acids and hydrocarbons
Chemical recycling of plastic wastes is of great significance for sustainable development, which also represents challenges and opportunities for synthesis of value-added chemicals. Here, the authors report a general strategy to degrade polyesters via directly breaking the C-O bond by nucleophilic substitution of halide anion of ionic liquids.
- Wei Zeng
- , Yanfei Zhao
- & Zhimin Liu
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Article
| Open AccessHighly scalable photoinduced synthesis of silanols via untraversed pathway for chlorine radical (Cl•) generation
Contrary to photocatalysis, the use of photochemical energy solely to initiate reactions is underexplored. Here, the authors demonstrate light initiated synthesis of functionalized organosilanols, silanediols, and polymeric siloxanol under ambient reaction conditions.
- Argha Saha
- , Wajid Ali
- & Debabrata Maiti
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Article
| Open AccessTotal wash elimination for solid phase peptide synthesis
Peptide drug manufacturing commonly uses large amounts of hazardous solvents primarily due to multiple washings after each step. Here, the authors introduce the concept of a completely wash-free methodology that enables up to 95% waste reduction.
- Jonathan M. Collins
- , Sandeep K. Singh
- & Christopher L. Houser
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Article
| Open AccessWood-based superblack
Superblack materials could innovate light-centered technologies, however, advances in superblack materials have been constrained by their complex and costly fabrication routes. Here, the authors report a simple top-down strategy, guided by computational methods, to develop robust superblack materials following metal-free wood delignification and carbonization.
- Bin Zhao
- , Xuetong Shi
- & Bruno D. Mattos
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Article
| Open AccessStraightforward synthesis of functionalized γ-Lactams using impure CO2 stream as the carbon source
Direct utilization of CO2 is important in organic synthesis but purification of CO2 gas expensive and energy intensive. Here the authors described a straightforward synthetic route for the synthesis of γ-lactams, a pivotal core structure of bioactive molecules, by using impure CO2 stream as the carbon source.
- Yuman Qin
- , Robin Cauwenbergh
- & Shoubhik Das
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Article
| Open AccessPulsed electroreduction of low-concentration nitrate to ammonia
Electrocatalytic nitrate reduction to ammonia has emerged as an alternative strategy for effluent treatment and ammonia production. Here, the authors report a pulsed potential approach to overcome the sluggish reaction kinetics caused by the limited distribution of negatively charged nitrate near the working electrode and the competing side reactions.
- Yanmei Huang
- , Caihong He
- & Yifu Yu
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Article
| Open AccessControlling the selectivity of the hydrogenolysis of polyamides catalysed by ceria-supported metal nanoparticles
Converting waste plastic into valuable chemicals is of high interest. However, transformation of N-containing polymers is still challenging. Here the authors report hydrogenolysis of various polyamides using Pt-group metal supported on CeO2 with different selectivity of the alkane using varied Pt-group metals.
- XinBang Wu
- , Wei-Tse Lee
- & Paul J. Dyson
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Article
| Open AccessEnergy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering
The development of robust catalysts that could work under industrial-scale current densities bring promise but also a challenge for hydrogen production. Here, the authors report an in situ activation method to produce ferromagnetic ruthenium clusters that can catalyze the hydrogen evolution reaction at high current densities.
- Jun Qi
- , Yadong Du
- & Jieshan Qiu
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Article
| Open AccessTowards bioresource-based aggregation-induced emission luminogens from lignin β-O-4 motifs as renewable resources
Biorenewable feedstocks are important for developing more sustainable materials, but developing processes can be challenging due to incompatible reaction conditions. Here, the authors report the one-pot preparation of aggregation-induced emission luminogens from lignin moieties.
- Tenglong Guo
- , Yuting Lin
- & Tao Zhang
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Article
| Open AccessIron phosphide nanocrystals as an air-stable heterogeneous catalyst for liquid-phase nitrile hydrogenation
Iron is an ideal catalytic material due to its abundance, low cost, and low toxicity, but conventional iron catalysts show low activity and lack air stability. Here, the authors report an iron phosphide nanocrystal catalyst, which exhibits high stability in air and high activity for the liquid-phase nitrile hydrogenations.
- Tomohiro Tsuda
- , Min Sheng
- & Takato Mitsudome
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Article
| Open AccessSolar-driven upgrading of biomass by coupled hydrogenation using in situ (photo)electrochemically generated H2
Green chemical transformations driven by renewable energies are imperative to realize a sustainable energy society. We demonstrate a coupled approach to hydrogenate biomass feedstock into valuable chemicals with high stability using hydrogen generated in situ in a (photo)electrochemical reactor.
- Keisuke Obata
- , Michael Schwarze
- & Fatwa F. Abdi
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Article
| Open AccessAnionic ring-opening polymerization of functional epoxide monomers in the solid state
Despite recent advancements in mechanochemical polymerization, understanding the unique mechanochemical reactivity during the ball milling polymerization process still requires extensive investigations. Here the authors use solid-state anionic ring-opening polymerization to synthesize polyethers from various functional epoxide monomers.
- Jihye Park
- , Ahyun Kim
- & Byeong-Su Kim
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Article
| Open AccessThe isocyanide SN2 reaction
The nucleophilic substitution reaction (SN2) is one of the oldest yet very useful organic transformations, but surprisingly, the nucleophilic character of isocyanides has never been explored in SN2 reactions. Here the authors show that isocyanides react as versatile nucleophiles in SN2 reactions with alkyl halides in a general manner to afford highly substituted secondary amides by in situ hydrolysis of the intermediate nitrilium ion.
- Pravin Patil
- , Qiang Zheng
- & Alexander Dömling
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Article
| Open AccessAtomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading
Electrocatalytic conversion of low-cost organic compounds to high-value chemicals urgently demands the development of efficient electrocatalysts. Mao et al. report the synthesis of Cu single-atom dispersed Rh metallene arrays for electrochemical aniline synthesis and biomass upgrading with enhanced electrocatalytic activity.
- Qiqi Mao
- , Xu Mu
- & Hongjing Wang
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Article
| Open AccessScalable electrosynthesis of commodity chemicals from biomass by suppressing non-Faradaic transformations
Electrooxidation of biomass provides a sustainable route to produce valuable chemicals, but suffers from non-Faradaic degradation in alkaline electrolysis at high reactant concentration. Here, the authors develop a single-pass continuous flow reactor to tackle this challenge, achieving kilogram-scale and continuous electrooxidation of glucose to formate and 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid with high selectivity and high concentration.
- Hua Zhou
- , Yue Ren
- & Haohong Duan
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Article
| Open AccessHydrogenation of different carbon substrates into light hydrocarbons by ball milling
Conventional methods to gasify or liquefy carbon-based polymers use high temperatures because of carbon–carbon bond stability. Here, the authors describe a mechanochemical ball milling method to break carbon–carbon bonds without heating.
- Linfeng Li
- , Olena Vozniuk
- & Ferdi Schüth
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Article
| Open AccessUnderstanding catalytic synergy in dinuclear polymerization catalysts for sustainable polymers
Understanding the intermetallic synergy and the structure-performances relationships of catalysts remains challenging. Here, the authors demonstrate a relationship between both the rates, selectivity and the s-block metal acidity in a series of heterodinuclear catalysts based on Co(III) in combination with alkali and alkaline earth metals for three different polymerization reactios.
- Francesca Fiorentini
- , Wilfred T. Diment
- & Charlotte K. Williams
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Article
| Open AccessTransforming sustainable plant proteins into high performance lubricating microgels
Demand for plant proteins is increasing, but these often give an astringent sensation due to poor lubrication performance. Here, the authors report the development of plantprotein microgels with improved lubricity with potential in sustainable foods.
- Ben Kew
- , Melvin Holmes
- & Anwesha Sarkar
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Article
| Open AccessHydrogenation versus hydrogenolysis during alkaline electrochemical valorization of 5-hydroxymethylfurfural over oxide-derived Cu-bimetallics
Electrochemical conversion of biomass emerges as a green alternative to high pressure, high temperature and hazardous equivalents from classical organic chemistry. Here, the authors show that the electrochemical hydrogenolysis can prevail over the hydrogenation under strong alkaline conditions.
- Philipp Hauke
- , Thomas Merzdorf
- & Peter Strasser
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Article
| Open AccessModulating adsorbed hydrogen drives electrochemical CO2-to-C2 products
A dual-site catalyst consisting of Cu nanoparticles (NPs) and atomic Cu sites is designed. The atomic Cu boosts H2O dissociation for modulating the *H coverage on Cu NPs, improving the efficiency of CO2 electroreduction to multi-carbon products.
- Jiaqi Feng
- , Libing Zhang
- & Buxing Han
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Article
| Open AccessPhotocatalytic conversion of sugars to 5-hydroxymethylfurfural using aluminium(III) and fulvic acid
5-hydroxymethylfurfural (HMF) is an essential platform chemical for developing a sustainable fine-chemical industry but cost-effective production of HMF requires mild reaction temperatures and efficient catalysts. Here, the authors report a fulvic acid Al complex with photocatalytic activity under sunlight for glucose conversion to HMF in one-pot reaction with good yield.
- Tana Tana
- , Pengfei Han
- & Huai-Yong Zhu
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Comment
| Open AccessDirect synthesis of urea from carbon dioxide and ammonia
Urea, a crucial nitrogen fertilizer, plays a vital role in meeting global food demand. However, its current production method is energy-intensive and environmentally unfriendly. In this commentary article, the authors propose strategies to address and overcome these challenges.
- Jie Ding
- , Runping Ye
- & Maohong Fan
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Article
| Open AccessEnhancing polyol/sugar cascade oxidation to formic acid with defect rich MnO2 catalysts
This work develops defective MnO2 catalysts with Frustrated Lewis Pairs through a coordination number reduction strategy to enhance the aerobic oxidation of various polyols/sugars to formic acid.
- Hao Yan
- , Bowen Liu
- & Ning Yan
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Article
| Open AccessPhotothermal recycling of waste polyolefin plastics into liquid fuels with high selectivity under solvent-free conditions
Sustainable recycling of waste plastics is of highly strategic significance. Here, the authors report a photothermal recycling system for transforming polyolefin plastics into high-selectivity liquid fuels through the synergistic utilization of ultraviolet, visible, and near-infrared irradiation.
- Yingxuan Miao
- , Yunxuan Zhao
- & Tierui Zhang
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Article
| Open AccessA sodium-ion-conducted asymmetric electrolyzer to lower the operation voltage for direct seawater electrolysis
Hydrogen produced directly from neutral seawater is promising but challenging due to seawater’s complex composition. Here, the authors report a Na+-conducted pH-asymmetric electrolyzer that can directly split seawater into hydrogen with low electricity cost and nearly zero chloride interference.
- Hao Shi
- , Tanyuan Wang
- & Qing Li
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Article
| Open AccessCarbon neutral hydrogen storage and release cycles based on dual-functional roles of formamides
The search for new carbon-based hydrogen storage materials attracts scientists from various disciplines. Now, carbon-neutral hydrogen storage-release is reported based on dual-functional roles of formamides and uses non-noble, Fe-based catalyst.
- Duo Wei
- , Xinzhe Shi
- & Matthias Beller
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Article
| Open AccessSolution-processable polymers of intrinsic microporosity for gas-phase carbon dioxide photoreduction
This works presents a series of solution processable, conjugated polymers of intrinsic microporosity, which are used as photocatalysts for carbon dioxide reduction to carbon monoxide in the presence of hydrogen.
- Floriana Moruzzi
- , Weimin Zhang
- & Iain McCulloch
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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 AccessInsights into substitution strategy towards thermodynamic and property regulation of chemically recyclable polymers
The global plastic pollution crisis can be mitigated by developing chemically recyclable polymers following the monomer design principle. Here, the authors evaluate substitution effects and structure−property relationships in the ɛ-caprolactone system to guide the design of monomers for the preparation of chemically recyclable polymers.
- Yi-Min Tu
- , Fu-Long Gong
- & Jian-Bo Zhu
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Article
| Open AccessElectrosynthesis of a nylon-6 precursor from cyclohexanone and nitrite under ambient conditions
The sustainable synthesis of cyclohexanone oxime, the precursor of nylon-6, without toxic SO2 or H2O2 usage is desirable. Here, the electrosynthesis of cyclohexanone oxime from nitrite and cyclohexanone under ambient conditions is reported.
- Yongmeng Wu
- , Jinghui Zhao
- & Bin Zhang
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Article
| Open AccessDirect conversion of lignin to functionalized diaryl ethers via oxidative cross-coupling
Efficient valorization of lignin, a sustainable source of functionalized aromatic products, would reduce dependence on fossil-derived feedstocks. Here, the authors directly transform lignin into valuable functionalized diaryl ethers in near-theoretical-maximum yields, using oxidative cross coupling under copper catalysis.
- Mingyang Liu
- & Paul J. Dyson
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Article
| Open AccessWater decontamination via nonradical process by nanoconfined Fenton-like catalysts
There is an urgent need to develop effective heterogeneous Fenton-like catalysts for water treatment. Here, the authors demonstrate that nanoconfinement of cobalt oxide catalysts in carbon nanotubes can selectively degrade pollutants at high reaction rate.
- Tongcai Liu
- , Shaoze Xiao
- & Yalei Zhang