Featured
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| Open AccessDirect synthesis of oxalic acid via oxidative CO coupling mediated by a dinuclear hydroxycarbonylcobalt(III) complex
Oxidative coupling of CO is a straightforward but currently underdeveloped economically benign synthetic route to target α-diketones. Here, the authors synthesize a rare coplanar dinuclear hydroxycarbonylcobalt(III) complex and demonstrate that the Co – carboxylate bonds can be easily cleaved leading to the formation of oxalic acid.
- Yingzhuang Xu
- , Songyi Li
- & Huayi Fang
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Article
| Open AccessRoom temperature phosphorescence from natural wood activated by external chloride anion treatment
Converting natural wood to room temperature phosphorescent (RTP) materials is a complex process often requiring toxic reagents. Here the authors convert natural wood to a RTP material using external chloride ions from a MgCl2 solution, obtaining a promising luminescent additive material for 3D printing.
- Yingxiang Zhai
- , Shujun Li
- & Zhijun Chen
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Article
| Open AccessRegulation of molecular transport in polymer membranes with voltage-controlled pore size at the angstrom scale
The ability to regulate membrane pore size as needed has been a topic of active research for developing next-generation stimuli-responsive smart membranes. Herein, the authors report the observation of operando regulation of the pore size of A membrane based on electro-osmotic swelling.
- Yuzhang Zhu
- , Liangliang Gui
- & Jian Jin
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Article
| Open AccessA selective and atom-economic rearrangement of uridine by cascade biocatalysis for production of pseudouridine
Pseudouridine (Ψ), the C-nucleoside isomer of uridine, and its 1-N-methyl derivative, are incorporated in mRNA vaccines and essential for their efficiency, but difficult to synthetically access. Here, the authors report on selective and atom-economic 1N-5C rearrangement of β-d-ribosyl on uracil to obtain Ψ from unprotected U in quantitative yield
- Martin Pfeiffer
- , Andrej Ribar
- & Bernd Nidetzky
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Article
| Open AccessElectrochemical oxidative difunctionalization of diazo compounds with two different nucleophiles
The difunctionalization of diazo compounds, traditionally with one nucleophile and one electrophile, is a powerful strategy. Here, the authors develop a path of electrochemical oxidative difunctionalization of diazo compounds with two different nucleophiles.
- Dongfeng Yang
- , Zhipeng Guan
- & Aiwen Lei
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Article
| Open AccessMixed-valence molybdenum oxide as a recyclable sorbent for silver removal and recovery from wastewater
Silver ions in wastewater are a major health hazard, and there is an urgent need to develop methods to reliably extract them. Here, the authors show that mixed-valence molybdenum oxide can selectively adsorb and reduce Ag+ from wastewater and be easily recycled while maintaining high selectivity towards Ag+.
- Penghui Shao
- , Ziwen Chang
- & Liming Yang
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Article
| Open AccessTurning dead leaves into an active multifunctional material as evaporator, photocatalyst, and bioplastic
Large numbers of leaves fall off trees each autumn. Here, the authors turn dead leaves into an active material which acts as bioplastic and shows high performance in solar water evaporation, photocatalytic H2 production and antibiotic degradation.
- Siyuan Fang
- , Xingyi Lyu
- & Yun Hang Hu
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Article
| Open AccessIn-situ forming dynamic covalently crosslinked nanofibers with one-pot closed-loop recyclability
Polymeric nanofibers are attractive nanomaterials owing to their high surfacearea- to-volume ratio and superior flexibility but designing durable and recyclable polymer nanofibers is challenging. Here, the authors integrate the concept of covalent adaptable networks to produce dynamic covalently crosslinked nanofibers via electrospinning.
- Sheng Wang
- , Nannan Wang
- & Zibiao Li
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Article
| Open AccessDesigning covalent organic frameworks with Co-O4 atomic sites for efficient CO2 photoreduction
A class of inexpensive aminoanthraquinone organic dyes are shown to facilitate visible-light-driven CO2 reduction. Overall reaction efficiencies were found to be optimal when both electron donating and accepting groups were on a single dye molecule.
- Qian Zhang
- , Shuaiqi Gao
- & Jianji Wang
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Article
| Open AccessOxidation of metallic Cu by supercritical CO2 and control synthesis of amorphous nano-metal catalysts for CO2 electroreduction
Amorphous metal catalysts often exhibit appealing catalytic properties, however, accurate control synthesis of amorphous nano-metal catalysts is a challenge. Here, the authors report a feasible strategy to prepare the amorphous Cu catalysts by supercritical CO2 treatment followed by electroreduction. The resulted catalyst shows high selectivity towards multi-carbon products for CO2 electroreduction.
- Chunjun Chen
- , Xupeng Yan
- & Buxing Han
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Article
| Open AccessRenewable formate from sunlight, biomass and carbon dioxide in a photoelectrochemical cell
The sustainable production of chemicals and fuels from waste carbon sources holds significant promise for reducing our dependence on fossil resources. Here, the authors demonstrate renewable formate production from biomass wastes and CO2 powered by solar energy.
- Yuyang Pan
- , Huiyan Zhang
- & Sheng Chu
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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 AccessRational design of N-heterocyclic compound classes via regenerative cyclization of diamines
Introducing unknown compound classes is the key to extent the chemical space qualitatively. Here the authors report on a concept to design heterocyclic compound classes rationally and the synthesis of unknown classes of N-heterocyclic compounds
- Robin Fertig
- , Felix Leowsky-Künstler
- & Rhett Kempe
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Article
| Open AccessStabilizing copper sites in coordination polymers toward efficient electrochemical C-C coupling
Typically, Cu catalysts agglomerate under electrochemical conditions. Here, the authors report a coordination polymer catalyst with neighboring Cu sites which remain isolated and reduce CO2 to C2H4 with high selectivity and stability
- Yongxiang Liang
- , Jiankang Zhao
- & Jie Zeng
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Article
| Open AccessSelective photoelectrochemical oxidation of glucose to glucaric acid by single atom Pt decorated defective TiO2
Photoelectrochemical oxidation provides a promising strategy for glucaric acid production. Here, selective oxidation of glucose to glucaric acid is realized on the photoanode of defective TiO2 decorated with single-atom Pt via a photoelectrochemical strategy.
- Zhangliu Tian
- , Yumin Da
- & Wei Chen
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Article
| Open AccessOvercoming the low reactivity of biobased, secondary diols in polyester synthesis
Glucose-derived isosorbide is a rigid polyester monomer with a low reactivity. Here, the authors report the synthesis of high molecular weight biobased polyesters with promising barrier and mechanical properties via in situ generation of reactive aryl ester groups.
- Daniel H. Weinland
- , Kevin van der Maas
- & Gert-Jan M. Gruter
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Article
| Open AccessRegulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene
Developing highly efficient catalysts for selective oxidation of benzene to phenol with low H2O2 consumption remains challenging. Here the authors report a highly active and selective non-noble metal catalyst for selective oxidation of benzene to phenol with low H2O2 addition via regulating the electron configuration of single-atom Cu catalyst.
- Ting Zhang
- , Zhe Sun
- & Zhongkui Zhao
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Article
| Open AccessAqueous synthesis of highly functional, hydrophobic, and chemically recyclable cellulose nanomaterials through oxime ligation
Water is a standing challenge in the chemical modification of cellulose nanofibrils. Here, authors employ oxime-ligation to solve this by direct covalent chemistry on dialdehyde-CNF in water and assess the material for potential applications in green electronics and triboelectric nanogenerators.
- Elena Subbotina
- , Farsa Ram
- & Peter Olsén
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Article
| Open AccessOne-pot H/D exchange and low-coordinated iron electrocatalyzed deuteration of nitriles in D2O to α,β-deuterio aryl ethylamines
One-pot efficient synthesis of α,β-deuterio aryl ethylamines with high deuterium ratios using an easy-to-handle deuterated source under ambient conditions is desirable. Here the author report the electrosynthesis of α,β-deuterio aryl ethylamines from aryl acetonitriles using D2O.
- Rui Li
- , Yongmeng Wu
- & Bin Zhang
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Article
| Open AccessSolar reduction of carbon dioxide on copper-tin electrocatalysts with energy conversion efficiency near 20%
Solar-driven carbon dioxide reduction has witnessed a renaissance in the past decades, but the system suffers from low reaction rates. Here the authors develop a copper/tin-oxide electrocatalyst, achieving a new benchmark solar-to-CO energy conversion efficiency in a flow electrolyzer.
- Jing Gao
- , Jun Li
- & Michael Grätzel
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Article
| Open AccessHighly reinforced and degradable lignocellulose biocomposites by polymerization of new polyester oligomers
Cellulose biocomposites from nanocellulose or plant fibers with polymer matrix are often not degradable and suffer from insufficient mechanical properties to replace established materials. Here, the authors demonstrate the fabrication of hydrolytically degradable polymers through in-situ polymerization of new functionally balanced oligomers within high-content lignocellulose reinforcement networks.
- Erfan Oliaei
- , Peter Olsén
- & Lars A. Berglund
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Article
| Open AccessMain-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution
The introduction of hydrophilic segments into the main-chain of polymer photocatalysts allows water to efficiently enter the interior through these hydrophilic segments, and results in effective water/polymer interfaces for hydrogen evolution.
- Chih-Li Chang
- , Wei-Cheng Lin
- & Ho-Hsiu Chou
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Article
| Open AccessGrave-to-cradle upcycling of Ni from electroplating wastewater to photothermal CO2 catalysis
The valorization of undesirable substrates offers a two-fold strategy for pollution remediation and renewable energy conversion. Here, authors demonstrate the scavenging of Ni from electroplating wastewater and subsequent utilization as materials for photothermal CO2 reduction.
- Shenghua Wang
- , Dake Zhang
- & Geoffrey A. Ozin
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Article
| Open AccessEnvironmentally adaptive MOF-based device enables continuous self-optimizing atmospheric water harvesting
Atmospheric water harvesting by MOF-based devices is critically dependent on weather conditions. Here, the authors report a MOF-based adaptive water harvesting system capable of adapting its cycles to temperature and relative humidity fluctuations throughout the day, continuously optimizing water production.
- Husam A. Almassad
- , Rada I. Abaza
- & Kyle E. Cordova
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Article
| Open AccessMechanistic classification and benchmarking of polyolefin depolymerization over silica-alumina-based catalysts
Product distributions have been used to classify the depolymerization pathways of polyolefins catalyzed by silica-alumina-based catalysts to construct an activity-mechanism map as a benchmarking tool to facilitate catalyst discovery.
- Wei-Tse Lee
- , Antoine van Muyden
- & Paul J. Dyson
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Article
| Open AccessMechanochemical synthesis of inverse vulcanized polymers
Inverse vulcanization is a process that enables to convert sulfur, a by-product of the petroleum industry, into polymers. Here the authors report a synthetic method of inverse vulcanization via mechanochemical synthesis; compared to thermal routes, a broader range of monomers can be used, and the protocol yields materials with enhanced mercury capture capacity.
- Peiyao Yan
- , Wei Zhao
- & Tom Hasell
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Article
| Open AccessCatalytic oxidation of polystyrene to aromatic oxygenates over a graphitic carbon nitride catalyst
There is a real need to create materials capable of plastic recycling and upcycling. Here, the authors report a heterogeneous carbon nitride photocatalyst which efficiently converts polystyrene plastics into aromatic oxygenates, such as benzoic acid.
- Ruochen Cao
- , Mei-Qi Zhang
- & Ding Ma
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Article
| Open AccessRational highly dispersed ruthenium for reductive catalytic fractionation of lignocellulose
Lignin valorization becomes the spotlight on the full utilization of biomass. Here, the authors report a highly dispersed Ru catalyst for reductive catalytic fractionation of lignocellulose, which affords monophenols in theoretical maximum yields, along with high preservation of carbohydrate.
- Zhenzhen Liu
- , Helong Li
- & Guoyong Song
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Article
| Open AccessSelective separation of light rare-earth elements by supramolecular encapsulation and precipitation
The separation of the rare-earth elements is a significant scientific challenge. Here, the authors report the selective precipitation of the light rare-earths as supramolecular capsules from acidic, industrially relevant, mixed-metal solutions.
- Joseph G. O’Connell-Danes
- , Bryne T. Ngwenya
- & Jason B. Love
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Article
| Open AccessA practical concept for catalytic carbonylations using carbon dioxide
Using CO2 as C1-feedstock for the chemical industry has attracted great attention. Here the authors develop a two-step cascade process to perform catalytic carbonylations of olefins, alkynes, and aryl halides using CO2 and H2.
- Rui Sang
- , Yuya Hu
- & Matthias Beller
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Comment
| Open AccessDifferences in barriers for controlled learning about safety between biotechnology and chemistry
In contrast to chemical industry, biotechnology is still not competitive for the production of chemicals, materials, and biofuels. Here, the authors discuss the underlying reasons and propose to address the problem through regulatory changes and risk management.
- Britte Bouchaut
- , Frank Hollmann
- & Lotte Asveld
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Article
| Open AccessSolvent-driven fractional crystallization for atom-efficient separation of metal salts from permanent magnet leachates
Rare earth elements are essential to electrified infrastructure and clean energy production. Here, authors show reagent- and energy-efficient separation of lanthanides from secondary feedstock using dimethyl ether-driven fractional crystallization.
- Caleb Stetson
- , Denis Prodius
- & Aaron D. Wilson
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Article
| Open AccessFacile and general electrochemical deuteration of unactivated alkyl halides
Deuterium-labelled compounds are useful for mechanistic studies and pharmaceutical science, but syntheses are not trivial. Here, the authors report deuteration of unactivated alkyl (pseudo)halides driven by electrochemical force, using deuterium oxide as the source of the isotope.
- Pengfei Li
- , Chengcheng Guo
- & Youai Qiu
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Article
| Open AccessDecoupling the electronic and geometric effects of Pt catalysts in selective hydrogenation reaction
Decoupling the electronic and geometric effects has been a long cherished goal for heterogeneous catalysis due to their tangled relationship. Here the authors propose a novel orthogonal decomposition method to decouple the electronic and geometric effect for supported metal catalysts.
- Zhe Wang
- , Chunpeng Wang
- & Yong Wang
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Article
| Open AccessFully lignocellulose-based PET analogues for the circular economy
‘Polyethylene terephthalate is a widely used polymer with a concerning environmental impact, and alternatives are now highly sought. In this article, the authors present a biorefinery strategy for constructing polyester analogues of polyethylene terephthalate from woody biomass, which are promising candidates for the circular economy.
- Xianyuan Wu
- , Maxim V. Galkin
- & Katalin Barta
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| Open AccessConverting waste PET plastics into automobile fuels and antifreeze components
To solve the serious problem of white plastic pollution many degradation routes are being investigated. Here the authors show a H2-free low-cost Cu/SiO2 catalyzed process to quantitatively convert polyethylene terephthalate into p-xylene and ethylene glycol in one pot with methanol as both the solvent and hydrogen source at 210 °C.
- Zhiwen Gao
- , Bing Ma
- & Chen Zhao
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Article
| Open AccessHierarchical micro/nanostructured silver hollow fiber boosts electroreduction of carbon dioxide
An activated silver hollow fiber electrode enables enhanced triphasic interface reactions and oriented mass transfers synergistically, facilitating efficient CO2 conversion (> 50%) to boost CO production with a current density of 1.26 A · cm−2.
- Shoujie Li
- , Wei Chen
- & Yuhan Sun
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Article
| Open AccessHighly stable and tunable peptoid/hemin enzymatic mimetics with natural peroxidase-like activities
Peroxidase mimics are currently being investigated as catalysts for lignin depolymerisation. In this article, the authors investigate a class of self-assembled and highly stable peptoid/hemin nanomaterials as peroxidase mimics that are highly stable and tuneable for the depolymerisation of a biorefinery lignin.
- Tengyue Jian
- , Yicheng Zhou
- & Chun-Long Chen
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Article
| Open AccessSynergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light
CH4 oxidation to high value chemicals under mild conditions through photocatalysis confronts critical issues regarding both conversion and selectivity. Here, atomic Pd and oxygen vacancies were integrated on In2O3 nanorods, leading to visible-driven CH4 conversion with a remarkable yield of oxygenates and high selectivity of primary products.
- Lei Luo
- , Lei Fu
- & Junwang Tang
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Article
| Open AccessCoordination environment tuning of nickel sites by oxyanions to optimize methanol electro-oxidation activity
Coordination environments around metal sites are important in electrocatalysis. Here, Ni metalloid oxidation produces oxyanion doped amorphous Ni-oxyhydroxides where substitution with phosphorus is found to boost methanol electrooxidation activity.
- Shanlin Li
- , Ruguang Ma
- & Jiacheng Wang
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Article
| Open AccessSubnanometric Cu clusters on atomically Fe-doped MoO2 for furfural upgrading to aviation biofuels
Single cluster catalysts are considered as versatile boosters in heterogeneous catalysis. Here the authors report subnanometric Cu clusters dispersed on Fe-doped MoO2 support exhibits attractive performance in furfural valorization to C8-C15 aviation biofuels via a newly developed reaction route.
- Xin Zhao
- , Fengliang Wang
- & Yingwei Li
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Article
| Open AccessSkeletal Ni electrode-catalyzed C-O cleavage of diaryl ethers entails direct elimination via benzyne intermediates
Biomass conversion holds promise as a more sustainable source of platform chemicals, but limitations in the ways in which lignin can be broken down is a current bottleneck. Here the authors report an electrocatalytic hydrogenolysis over skeletal Ni that cleaves diaryl ethers, chemically resistant moieties in both renewable carbon sources and persistent organic pollutants.
- Yuting Zhou
- , Grace E. Klinger
- & James E. Jackson
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Comment
| Open AccessAnalysing the relationship between the fields of thermo- and electrocatalysis taking hydrogen peroxide as a case study
Research in thermo- and electrocatalysis have often preceded in isolation, even for similar reactions. Here, the authors compare current trends in both fields and elaborate on the commonalities and differences with a specific focus on the production of hydrogen peroxide.
- Guilherme V. Fortunato
- , Enrico Pizzutilo
- & Marc Ledendecker
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Article
| Open AccessPressure-induced liquid-liquid transition in a family of ionic materials
Liquid−liquid transitions (LLTs) have been reported for some molecular systems but are difficult to observe under high pressure conditions. Here the authors report and characterize a first-order LLT in a series of ionic liquids containing the trihexyl(tetradecyl)phosphonium cation and anions of different sizes and shapes, using calorimetric and dielectric measurements.
- Zaneta Wojnarowska
- , Shinian Cheng
- & Marian Paluch
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Article
| Open AccessBiocatalysed synthesis planning using data-driven learning
As of now, only rule-based systems support retrosynthetic planning using biocatalysis, while initial data-driven approaches are limited to forward predictions. Here, the authors extend the data-driven forward reaction as well as retrosynthetic pathway prediction models based on the Molecular Transformer architecture to biocatalysis.
- Daniel Probst
- , Matteo Manica
- & Teodoro Laino
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Article
| Open AccessVisible light-driven efficient palladium catalyst turnover in oxidative transformations within confined frameworks
Pd(II) catalyst turnover by reoxidation of a low valent Pd species is the key step for a Pd(II) catalyzed oxidation reaction. Here, the authors report a new strategy to address Pd reoxidation by fabricating spatially proximate photocatalyst and Pd(II) catalyst into metal-organic framework.
- Jiawei Li
- , Liuqing He
- & Huanfeng Jiang
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Article
| Open AccessNon-thermal plasma-assisted rapid hydrogenolysis of polystyrene to high yield ethylene
Current recycling methods suffer from harsh reaction conditions and long reaction times. Here the authors show a non-thermal plasma-assisted method for rapid hydrogenolysis of polystyrene at ambient temperature and atmospheric pressure, generating high yield (>40 wt%) of C1–C3 hydrocarbons.
- Libo Yao
- , Jaelynne King
- & Zhenmeng Peng
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Article
| Open AccessUnraveling of cocatalysts photodeposited selectively on facets of BiVO4 to boost solar water splitting
Artificial photosynthesis offers an integrated means to convert light to fuel, but efficiencies are often low. Here, authors report a Z-scheme system utilizing Ir and FeCoOx co-catalysts to enhance charge separation on BiVO4 facets that achieves high quantum efficiencies for overall water splitting.
- Yu Qi
- , Jiangwei Zhang
- & Fuxiang Zhang
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Article
| Open AccessMerging enzymes with chemocatalysis for amide bond synthesis
Proteins, other metabolites and many valuable synthetic products contain amide bonds and there is a need for more sustainable amide synthesis routes. Here the authors show an integrated next generation multi-catalytic system, merging nitrile hydratase enzymes with a Cu-catalysed N-arylation reaction in a single reaction vessel, for the construction of ubiquitous amide bonds.
- Luis Bering
- , Elliott J. Craven
- & Jason Micklefield