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| Open AccessSurface fluorination of BiVO4 for the photoelectrochemical oxidation of glycerol to formic acid
This work reports a surface fluorination strategy to construct dynamic dual hydrogen bonds on semiconducting BiVO4 photoelectrode for glycerol oxidation to value-added C1 production formic acid in acidic solution.
- Yang Liu
- , Huishan Shang
- & Xu Xiang
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Article
| Open AccessMain-group compounds selectively activate natural gas alkanes under room temperature and atmospheric pressure
Activation of natural gas alkanes using main-group systems typically requires heating or photo-irradiation under high atmospheric pressure with low regioselectivity. Here the authors report Lewis acid-carbene adduct activation of C–H bonds in ethane, propane and n-butane under one atmospheric pressure and at room temperature with high selectivity.
- Runbo Pei
- , Wenju Chang
- & Xinping Wang
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Article
| Open AccessFully recyclable and tough thermoplastic elastomers from simple bio-sourced δ-valerolactones
While a large number of chemically recyclable thermoplastics have been developed in recent years, technologically bio-based and fully recyclable thermoplastic elastomers (TPEs) with excellent mechanical properties are lacking. Here the authors demonstrate an all δvalerolactone-based polyester tri-BCP TPEs, which exhibit not only closed-loop chemical recyclability but also exceptional toughness.
- Kai Ma
- , Hai-Yan An
- & Tie-Qi Xu
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Article
| Open AccessAmbient-pressure alkoxycarbonylation for sustainable synthesis of ester
Alkoxycarbonylation reactions are widely used in the chemical industry, but their sustainability is often hindered by inefficient CO utilization. Here, the authors tackle the challenge by developing a sustainable and efficient carbonylation process for producing methyl propionate, achieving high CO utilization and regioselectivity.
- Bin Zhang
- , Haiyang Yuan
- & Graham J. Hutchings
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Article
| Open AccessElectrosynthesis of adipic acid with high faradaic efficiency within a wide potential window
Here, authors use a membrane electrode assembly is conducted to produce adipic acid with high faradaic efficiency and productivity at an industrially relevant current density, while achieving >50 hours stability.
- Xiang Liu
- , Yu-Quan Zhu
- & Haohong Duan
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Article
| Open AccessMultivalent Cu sites synergistically adjust carbonaceous intermediates adsorption for electrocatalytic ethanol production
This study proposes a multivalent Cu-based catalyst (Cu-TAPT) for electrocatalytic CO2RR, which promotes specific intermediate formation by the synergy of Cu2+ and Cu+ sites, thereby achieving a 54.3% Faradaic efficiency of ethanol at 429 mA cm−2.
- Xiao Chen
- , Shuaiqiang Jia
- & Buxing Han
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Article
| Open AccessAggregation-induced C–C bond formation on an electrode driven by the surface tension of water
Electrochemical organic synthesis is typically conducted in organic media negatively affecting the sustainability of electrosynthesis. Here, the authors realize aggregation-driven electrochemical radical cross coupling of unsaturated compounds using only water as solvent.
- Mengfan Li
- & Xu Cheng
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Article
| Open AccessEnable biomass-derived alcohols mediated alkylation and transfer hydrogenation
Using carbonyl compounds or alcohols as alkylating reagents for the synthesis of α-alkylated nitriles is appealing from a sustainability perspective. Here, a single-atom catalyst with Zn–N4 motifs acting as Lewis acid sites effectively activates alcohols, thus promoting various alkylation and transfer hydrogenation reactions using biomass-derived alcohols as both the alkylating reagents and hydrogen donors.
- Xixi Liu
- , Liang Huang
- & Zehui Zhang
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Article
| Open AccessTailoring photocatalysts to modulate oxidative potential of anilides enhances para-selective electrochemical hydroxylation
Phenolic compounds have long captivated the interest of organic synthesis, particularly in their quest for selective hydroxylation of arenes using H2O as a hydroxyl source but the inherent high reactivity and low redox potential of phenols often lead to undesirable overoxidation byproducts. Here the authors develop an electrophotochemical approach, finetuning substrate oxidative potential and enabling para-selective hydroxylation of anilides.
- Jianye Zhang
- , Zhaoliang Yang
- & Aiwen Lei
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Article
| Open AccessPhotosynthesis of CH3OH via oxygen-atom-grafting from CO2 to CH4 enabled by AuPd/GaN
The direct co-conversion of CH4 and CO2 into valuable chemicals has been a longstanding scientific pursuit. Here, the authors present a photo-driven process that reforms these greenhouse gases together to generate CH3OH and CO over AuPd/GaN.
- Hui Su
- , Jing-Tan Han
- & Chao-Jun Li
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Article
| Open AccessCatalyst-free selective oxidation of C(sp3)-H bonds in toluene on water
The anisotropic water interfaces provide an environment to drive various chemical reactions not seen in bulk solutions. Here the authors report that the oil-water interface activates and oxidizes C(sp3)-H bonds in toluene, yielding benzaldehyde with high selectivity and conversion under mild, catalyst-free conditions.
- Kyoungmun Lee
- , Yumi Cho
- & Siyoung Q. Choi
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Article
| Open AccessAmpere-level CO2 electroreduction with single-pass conversion exceeding 85% in acid over silver penetration electrodes
Suppression of the competing H2 evolution reaction in CO2 electroreduction in strong acids remains a considerable challenge. Here, authors report a silver-based electrode that enables CO2 conversion to CO exceeding 85% at ampere-level current densities in pH = 1 electrolytes.
- Shoujie Li
- , Xiao Dong
- & Wei Wei
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Article
| Open AccessEthylene electrosynthesis from low-concentrated acetylene via concave-surface enriched reactant and improved mass transfer
Electrocatalytic semihydrogenation of acetylene produces ethylene without petroleum, but is hindered by the need to preprocess coal-derived acetylene. Here the authors report concave carbon-supported Cu nanoparticles to enrich local acetylene concentration for ethylene electrosynthesis from low-concentrated raw coal-derived acetylene with a 91.7% FE at 420 mA cm−2.
- Fanpeng Chen
- , Li Li
- & Bin Zhang
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Article
| Open AccessDemethylation C–C coupling reaction facilitated by the repulsive Coulomb force between two cations
Carbon chain elongation (CCE) is normally carried out using either chemical catalysts or bioenzymes. Herein we demonstrate a catalyst-free approach to promote demethylation C–C coupling reactions for advanced CCE constructed with functional groups under ambient conditions.
- Xiaoping Zhang
- , Keke Huang
- & Huanwen Chen
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Article
| Open AccessRoom temperature catalytic upgrading of unpurified lignin depolymerization oil into bisphenols and butene-2
Despite numerous techniques for lignin depolymerization into mixtures of valuable monomers, methods for their upgrading into final products are scarce. Here the authors present an alternative approach whereby the target monomers are selectively and directly converted in unpurified mixtures into easily separable bisphenols and butene-2 under mild conditions.
- Elena Subbotina
- , Layra Rodrigues Souza
- & Paul Anastas
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Article
| Open AccessActive species in chloroaluminate ionic liquids catalyzing low-temperature polyolefin deconstruction
The catalytic conversion of polyolefins into gasoline-range alkanes requires a comprehensive understanding of the catalytically active species and their corresponding performance. Here the authors tackle this need by examining the nuclearity of the chloroaluminate ions and their interactions with reaction intermediates.
- Wei Zhang
- , Rachit Khare
- & Johannes A. Lercher
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Article
| Open AccessHighly efficient recycling of polyester wastes to diols using Ru and Mo dual-atom catalyst
Chemical recycling of polyester wastes is of great significance for sustainable development. Here the authors report a Ru and Mo dual-atom catalyst for reconstructing polyester wastes into diols in water under mild conditions.
- Minhao Tang
- , Ji Shen
- & Zhimin Liu
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Article
| Open AccessPhotoelectrochemical Fe/Ni cocatalyzed C−C functionalization of alcohols
Alcohols are ubiquitous molecules throughout the chemical sciences, making them highly attractive starting materials for creating new C − C bonds. Herein, a method for the photoelectrochemical C − C functionalization of various alcohols was developed.
- Long Zou
- , Rui Sun
- & Qingquan Lu
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Article
| Open AccessMicroenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O
Achieving a high Faradaic efficiency in the electrocatalytic deuteration of organics with D2O at large current densities is challenging due to the competing D2 evolution side reaction. Here the authors report the combined nanotip-enhanced electric field and surfactant-modified interface microenvironment enabled electrocatalytic deuteration of organics in D2O with an 80% FE at −100 mA cm−2.
- Meng He
- , Rui Li
- & Bin Zhang
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Article
| Open AccessElectrochemical synthesis of peptide aldehydes via C‒N bond cleavage of cyclic amines
Peptide aldehydes are an important class of biomolecules, playing essential roles in various living systems, and there is an ongoing demand for the efficient synthesis of peptide aldehydes. Herein, the authors report the electrooxidative ring-opening reaction via C‒N bond cleavage for the synthesis of unnatural peptide aldehydes.
- Xinyue Fang
- , Yong Zeng
- & Zhixiong Ruan
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Article
| Open AccessAtom-level interaction design between amines and support for achieving efficient and stable CO2 capture
An amine-support system has been introduced through atom-level design, achieving low regeneration energy, excellent cyclic stability, high capacity, and rapid kinetics, stemming from electron-level interactions preventing carbamate dehydration.
- Xin Sun
- , Xuehua Shen
- & Zuotai Zhang
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Article
| Open AccessArtificial cellulosic leaf with adjustable enzymatic CO2 sequestration capability
Developing artificial leaves is crucial for advancing Net Zero Future, but most artificial leaves rely on the use of metal or semiconductors catalysts that usually have a lower catalytic activity and selectivity compared to biocatalysts. Here the AUs report Ecoleaf, a biodegradable artificial leaf that mimics the controlled expansion and contraction of stomata and enables enzymic CO2 conversion.
- Xing Zhu
- , Chenxi Du
- & Bin He
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Article
| Open AccessAn effective and rapidly degradable disinfectant from disinfection byproducts
Here, authors highlight ecological risks of a widely used disinfectant, chloroxylenol, and identify a more efficient and safer alternative from halo-phenolic disinfection byproducts, 2,6-dichlorobenzoquinone. They leverage seawater’s slightly alkaline nature to enhance its degradability via hydrolysis.
- Jiarui Han
- , Wanxin Li
- & Xiangru Zhang
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Article
| Open AccessCO2 electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels
Efficient electroreduction of CO2 to multi-carbon products under strong acidic condition is highly challenging. Here, the authors demonstrate that combining microenvironment modulation and La doping effect could promote multicarbon products generation in acidic electrolyte.
- Jiaqi Feng
- , Limin Wu
- & Buxing Han
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Article
| Open AccessRecovery of europium from E-waste using redox active tetrathiotungstate ligands
Rare-earth elements (REEs) are vital to the modern economy, yet their mining poses both geopolitical and environmental challenges. Here, authors present a highly selective method for the recovery of europium from spent fluorescent lamps using redox active tetrathiotungstate ligands.
- Marie A. Perrin
- , Paul Dutheil
- & Victor Mougel
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Article
| Open AccessInternal water circulation mediated synergistic co-hydrolysis of PET/cotton textile blends in gamma-valerolactone
Recycling strategies for mixed plastics and textile blends currently aim for recycling only one of the components. Here the authors demonstrate a water coupling strategy to co-hydrolyze polyester/cotton textile blends into polymer monomers and platform chemicals.
- Shun Zhang
- , Wenhao Xu
- & Yu-Zhong Wang
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Article
| Open AccessIntegrated optimization modelling framework for low-carbon and green regional transitions through resource-based industrial symbiosis
This study reports a quantitative tool for resource-based industries aimed at supporting sustainable, low-carbon regional transitions. The results provide optimal transition paths over traditional methods, highlighting the need for cleaner technology and industrial symbiosis.
- Xin Xie
- , Hang Fu
- & Shanying Hu
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Article
| Open AccessSelective production of methylindan and tetralin with xylose or hemicellulose
Indan and tetralin are used as fuel additives and intermediates in the manufacture of many products, including thermal-stable jet fuel. Here the authors report a route for the synthesis of methylindan and tetralin by the hydrogenolysis of xylose or hemicellulose over a non-noble metal catalyst, followed by further reaction over zeolite H-ZSM-5. Reviewer recognition:
- Zhufan Zou
- , Zhenjie Yu
- & Ning Li
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Article
| Open AccessAll-natural 2D nanofluidics as highly-efficient osmotic energy generators
Researchers report a sustainable nanofluidic osmotic energy harvester made from natural montmorillonite clay nanosheets and recycled cellulose. Scaled-up films of 700 cm2 show power output of 8 W m−2 with stability over 30 days
- Jiadong Tang
- , Yun Wang
- & Tieyong Zuo
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Article
| Open AccessIn-situ low-temperature sulfur CVD on metal sulfides with SO2 to realize self-sustained adsorption of mercury
Efficient removal of gaseous mercury (Hg0) from industrial flue gas is commonly constrained by SO2. Here, authors propose an in-situ sulfur CVD method on metal sulfides that reverses the harmful effects of SO2, achieving self-sustained adsorption of Hg0 and breaking the capacity limitations.
- Qinyuan Hong
- , Haomiao Xu
- & Naiqiang Yan
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Article
| 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