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Perspective
| Open AccessEmerging trends in chiral inorganic nanomaterials for enantioselective catalysis
Considerable attention has been directed towards chiral nanocatalysts due to their significant role in facilitating asymmetric organic transformations. Here the authors highlight the recent advancements and notable examples in the field of chiral inorganic nanocatalysts.
- Si Li
- , Xinxin Xu
- & Chuanlai Xu
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Article
| Open AccessHighly defective ultra-small tetravalent MOF nanocrystals
Crystalline materials’ properties are highly dependent on their size. Here authors report a general synthesis of ultrasmall (4–6 nm) and highly defective Zr/Hf-Metal Organic Frameworks nanoparticles that present enhanced peptide hydrolysis performance.
- Shan Dai
- , Charlotte Simms
- & Christian Serre
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Article
| Open AccessPathway-divergent coupling of 1,3-enynes with acrylates through cascade cobalt catalysis
The development of divergent reaction pathways controlled by different ligands is a critical goal. Here the authors describe a cobalt-catalyzed strategy for cascade coupling of 1,3-enynes with two molecules of acrylates through three reaction modes.
- Heng Wang
- , Xiaofeng Jie
- & Fanke Meng
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Article
| Open AccessHighly efficient anion exchange membrane water electrolyzers via chromium-doped amorphous electrocatalysts
Modulating the electronic structure of active metal sites is crucial to enhance the activity of anion-exchange membrane water electrolyzers. Here, the authors elaborate Cr-doped amorphous metal oxide catalysts with excellent activity and stability.
- Sicheng Li
- , Tong Liu
- & Tao Yao
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Article
| Open AccessLate-stage meta-C–H alkylation of pharmaceuticals to modulate biological properties and expedite molecular optimisation in a single step
Installation of small aliphatic motifs within pharmaceuticals provides a medicinally relevant tool in drug discovery programmes. Here, the authors report a late-stage meta-C–H alkylation method facilitating the biological properties modulation of therapeutic agents.
- Lucas Guillemard
- , Lutz Ackermann
- & Magnus J. Johansson
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Article
| Open AccessElectric-field-assisted proton coupling enhanced oxygen evolution reaction
Manganese complexes have long been utilized by nature to catalyze the oxygen evolution reaction (OER) but mirroring their efficiency in artificial electrochemical systems has proven difficult. This study centers on alpha-manganese dioxide (α-MnO2), which closely mimics natural MnIV-O-MnIII-HxO motifs, presenting a novel method for manipulating proton coupling within the OER process using an external electric field.
- Xuelei Pan
- , Mengyu Yan
- & Liqiang Mai
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Article
| Open AccessNoncovalent interaction with a spirobipyridine ligand enables efficient iridium-catalyzed C–H activation
Exploitation of noncovalent interactions has received much attention for the design of metal catalysts. However, because of the weak nature, CH-π interactions have been less utilized for the control of organic reactions. Here, the authors report that the CH-π interaction can be used to kinetically accelerate catalytic C-H activation of arenes.
- Yushu Jin
- , Boobalan Ramadoss
- & Laurean Ilies
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Article
| Open AccessPhotocatalytic Z/E isomerization unlocking the stereodivergent construction of axially chiral alkene frameworks
The stereospecific Z/E isomerization of tetrasubstituted alkenes remains underdeveloped, thus lacking in a stereodivergent synthesis of axially chiral alkenes. Here, authors report the atroposelective synthesis of tetrasubstituted alkene analogues by asymmetric allylic substitution-isomerization, followed by the photocatalyzed Z/E isomerization.
- Jie Wang
- , Jun Gu
- & Ying He
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Article
| Open AccessNanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation
The poisoning of single-atom catalysts hampers their performance. Here, the authors propose Au nanoparticles as an antidote for poisoned Au single-atom catalysts, with trace addition shown to reinforce and sustain propylene epoxidation.
- Qianhong Wang
- , Keng Sang
- & Xuezhi Duan
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Article
| Open AccessElectrocatalytic hydrogenation of acetonitrile to ethylamine in acid
Proton exchange membrane electrolyzers hold promise for ethylamine synthesis from acetonitrile, yet local acidity fosters proton reduction. Here, authors systematically screen metal catalysts, verifying their effectiveness in such electrolyzers.
- Chongyang Tang
- , Cong Wei
- & Xiangfeng Duan
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Article
| Open AccessSolvent-free selective hydrogenation of nitroaromatics to azoxy compounds over Co single atoms decorated on Nb2O5 nanomeshes
Single atom catalysts can endow exceptional activity and selectively. Here, the authors report a single atom Co catalyst and reveal the importance of geometric and electronic properties for synthesizing azoxy compounds under solvent-free conditions.
- Zhijun Li
- , Xiaowen Lu
- & Yu Wang
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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 AccessOrganocatalytic desymmetrization provides access to planar chiral [2.2]paracyclophanes
Planar chiral [2.2]paracyclophanes have a wide range of applications in asymmetric synthesis and materials science. However, they are accessed via time-consuming chiral separations or kinetic resolution approaches. Here, the authors report a simple, metal-free protocol for organocatalytic desymmetrization of prochiral diformyl[2.2]paracyclophanes.
- Vojtěch Dočekal
- , Filip Koucký
- & Jan Veselý
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Article
| Open AccessThermally stable Ni foam-supported inverse CeAlOx/Ni ensemble as an active structured catalyst for CO2 hydrogenation to methane
An inverse CeAlOx/Ni/Ni-foam structured catalyst with high thermal stability and water resistance is shown to be effective at CO2 methanation across a wide temperature range because of efficient heat/mass transport.
- Xin Tang
- , Chuqiao Song
- & Lili Lin
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Article
| Open AccessReverse water gas-shift reaction product driven dynamic activation of molybdenum nitride catalyst surface
Catalyst activation commonly occurs during reactions. This study demonstrates that the surface’s active structure in nitride catalysts during the reverse water gas-shift reaction varies with the partial pressure of reaction products, resulting in enhanced catalytic activity through positive feedback between catalytic activity and the evolution of MoNx’s active structure.
- Hui Xin
- , Rongtan Li
- & Xinhe Bao
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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 AccessWater-assisted oxidative redispersion of Cu particles through formation of Cu hydroxide at room temperature
Redispersion of sintered metal species requires high temperatures in reactive atmospheres. Here, the authors report room temperature redispersion of supported Cu particles via formation of mobile hydroxylated Cu species induced by gaseous H2O and anchoring of the Cu species by surface OH groups.
- Yamei Fan
- , Rongtan Li
- & Qiang Fu
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Article
| Open AccessUpgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis
The transformation of CO2 with renewable hydrogen into high-value products presents a sustainable route for net-zero chemical manufacture. Here the authors introduce a LaFeO3 perovskite-mediated tandem conversion of CO2, achieving remarkable performance by separating the CO2 hydrogenation and C-C coupling domains in the catalyst system.
- Guo Tian
- , Zhengwen Li
- & Fei Wei
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Article
| Open AccessTumor-activated in situ synthesis of single-atom catalysts for O2-independent photodynamic therapy based on water-splitting
The utility of single-atom catalysts (SACs) for photodynamic therapy (PDT) has been limited by tumor hypoxia and side effects on normal tissues. Here the authors address these issues by developing an approach of tumor microenvironment-activated in situ synthesis of SACs for tumor-specific water-based PDT.
- Yiyan Yin
- , Xiyang Ge
- & Na Na
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Article
| Open AccessA silicon photoanode protected with TiO2/stainless steel bilayer stack for solar seawater splitting
Here, the authors report a Si photoanode coated with a TiO2/stainless steel bilayer to inhibit chloride adsorption and facilitate stable alkaline seawater splitting for over 50 h with an applied bias photon-to-current efficiency of 2.62%.
- Shixuan Zhao
- , Bin Liu
- & Jinlong Gong
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Article
| Open AccessEfficient bubble/precipitate traffic enables stable seawater reduction electrocatalysis at industrial-level current densities
Seawater electroreduction is a promising technique for producing hydrogen, but it is hindered by cathodic Mg2 + /Ca2+ precipitation. Here, the authors propose a microscopic bubble/precipitate traffic system that releases small-sized bubbles across the cathode to repel Mg2 + /Ca2+ precipitates from almost the entire surface area of the catalyst.
- Jie Liang
- , Zhengwei Cai
- & Bo Tang
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Article
| Open AccessPaired electrocatalysis unlocks cross-dehydrogenative coupling of C(sp3)-H bonds using a pentacoordinated cobalt-salen catalyst
Cross-dehydrogenative coupling (CDC) of C-H bonds is an ideal approach for C-C bond construction but suffers from low selectivity of similar C-H bonds. Here, the authors describe a highly selective paired electrocatalysis strategy towards CDC combining hydrogen evolution reaction catalysis with hydride transfer catalysis.
- Ke Liu
- , Mengna Lei
- & Sheng Zhang
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Article
| Open AccessTrialkoxysilane-Induced Iridium-Catalyzed para-Selective C–H Bond Borylation of Arenes
Controlling regioselectivity is one of the most challenging aspects for the construction of aryl boron compounds, and there are few practical and general strategies for such transformations. Here, the authors report an iridium-catalyzed trialkoxysilane protecting group-assisted regioselective C–H borylation with various aromatic compounds.
- Guodong Ju
- , Zhibin Huang
- & Yingsheng Zhao
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Article
| Open AccessJanus electronic state of supported iridium nanoclusters for sustainable alkaline water electrolysis
The hydrogen spillover effect improves the efficiency of the H2 evolution reaction but is incompatible with the O2 evolution reaction in alkaline water electrolysis. Here, the authors show that the Janus electronic state of supported Ir nanoclusters can couple hydrogen spillover and O2 evolution.
- Yaoda Liu
- , Lei Li
- & Zhengfei Dai
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Article
| Open AccessCarbon redirection via tunable Fenton-like reactions under nanoconfinement toward sustainable water treatment
Regulating the carbon evolution pathway during chemical oxidation is critical, but challenging, for sustainable water treatment. Here, the authors report an adaptive approach to drive carbon redirection from molecular fragmentation to polymerization under tunable nanoconfinement.
- Xiang Gao
- , Zhichao Yang
- & Bingcai Pan
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Article
| Open AccessDefect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
Converting nitrate to ammonia in wastewater with a wide range of nitrate concentrations remains a challenging task. Here the authors report defect-rich Cu nanowire electrocatalyst which can achieve 50 to 1100 mA cm−2 and over 90% Faradaic efficiency using 1–100 mM nitrate wastewater.
- Bocheng Zhang
- , Zechuan Dai
- & Genqiang Zhang
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Article
| Open AccessStereoselective assembly of C-oligosaccharides via modular difunctionalization of glycals
C-oligosaccharides are found in natural products and drug molecules, but their synthesis is challenging. Here, the authors report a strategy for the stereoselective and efficient synthesis of Coligosaccharides via palladium-catalyzed nondirected C1–H glycosylation/C2-alkenylation, cyanation, and alkynylation of 2-iodoglycals with glycosyl chloride donors.
- Ya-Nan Ding
- , Mei-Ze Xu
- & Yong-Min Liang
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Article
| Open AccessElectroreduction of unactivated alkenes using water as hydrogen source
The reduction of unactivated alkyl alkenes is a difficult challenge in organic chemistry. Here, the authors present a silicon-mediated electroreduction of alkyl alkenes, using water as a hydrogen source, enabled by [Fe]-H.
- Yanwei Wang
- , Qian Wang
- & Youai Qiu
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Article
| Open AccessPhoto-modulated activation of organic bases enabling microencapsulation and on-demand reactivity
Oil-water emulsion techniques can be used for encapsulation of chemicals and control of reactivity, but is challenging for highly reactive materials such as acids and bases. Here, the authors report the encapsulation of bases by masking of reactivity with photo-removable protecting groups.
- Wenle Li
- , Xiaocun Lu
- & Nancy R. Sottos
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Article
| Open AccessChiral BINOL-phosphate assembled single hexagonal nanotube in aqueous solution for confined rearrangement acceleration
Supramolecular confined catalysis aims to mimic the active pocket of an enzyme to enhance the efficiency and selectivity of catalytic reactions. Here, the authors describe the formation of chiral nanotubes stable in aqueous solution employing a chiral BINOL-phosphate which can accelerate the 3-aza-Cope rearrangement by a nanotubular interior confinement effect.
- Kang Li
- , Wei-Min Qin
- & Yue-Peng Cai
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Article
| Open AccessTailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer
The rational design of carbon-supported transition metal single atom catalysts with precise coordination tailoring remains challenging. Here, the authors develop a topological heteroatom-transfer strategy to precisely control the P coordination in Co single atoms for hydrogen evolution.
- Sheng Qian
- , Feng Xu
- & Jingqi Tian
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Article
| Open AccessConstructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting
Establishing optimal metal-support interactions is crucial for creating efficient catalysts for water splitting. Here, stable Ti–O–Ru interface formation and minimal work function difference between Ru nanoparticles and non-stoichiometric Ti4O7 lead to exceptional bifunctional activity of Ru/Ti4O7 for both HER and OER across pH-universal environments, maintaining stable operation for 500 h.
- Sheng Zhao
- , Sung-Fu Hung
- & Shengjie Peng
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Article
| Open AccessRoom temperature 3D carbon microprinting
Three-dimensional carbon microstructures with ultra-high aspect ratios are grown with a facile process using a metal-free catalyst and low-power visible light at room temperature, unlocking applications in flexible sensors and beyond.
- Fernand E. Torres-Davila
- , Katerina L. Chagoya
- & Laurene Tetard
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Article
| Open AccessBioorthogonal photocatalytic proximity labeling in primary living samples
Studying subcellular proteomes in primary living cells is crucial for understanding health and disease. Here, the authors introduce CAT-S, a non-genetic method based on photocatalysis, enabling in situ deciphering of mitochondrial proteomes in primary cells from mouse tissues and human blood.
- Ziqi Liu
- , Fuhu Guo
- & Xinyuan Fan
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Article
| Open AccessUnderstanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane
Methane is a potent greenhouse gas, and its removal is critical. Here, the authors demonstrate that spatially separated Cu and acid sites in Cu/zeolites influence product distribution and efficiency for methane oxidation.
- Peipei Xiao
- , Yong Wang
- & Toshiyuki Yokoi
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Article
| Open AccessMetal free cross-dehydrogenative N-N coupling of primary amides with Lewis basic amines
While the homo N-N coupling of two NH moieties to form the hydrazide N-N bond is well developed, the crossdehydrogenative hetero N-N coupling remains unevolved. Here the authors present an efficient, PhI(OAc)2-mediated intermolecular N-N cross-coupling of primary benzamides with primary and secondary amines.
- Subban Kathiravan
- , Prakriti Dhillon
- & Ian A. Nicholls
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Article
| Open AccessKeto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water
Hydrogen peroxide photosynthesis is an important reaction that suffers from poor activity due to the high energy barrier of hydrogen extraction in water. Here, we report a keto-form anthraquinone framework that shows promising performance in alkaline conditions.
- Xiangcheng Zhang
- , Silian Cheng
- & Lizhi Zhang
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Article
| Open AccessSolar-driven sugar production directly from CO2 via a customizable electrocatalytic–biocatalytic flow system
Solar-driven artificial food synthesis from CO2 provides an approach to overcome the limitations of natural photosynthesis, but it is very challenging. Here, the authors report a hybrid electrocatalytic-biocatalytic flow system, coupling photovoltaics-powered electrocatalysis (CO2 to formate) with a five enzyme cascade platform (formate to sugar), which achieves conversion of CO2 to C6 sugar (L-sorbose) with a solar-to-food energy conversion efficiency of 3.5%.
- Guangyu Liu
- , Yuan Zhong
- & Yujie Xiong
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Article
| Open AccessWater-participated mild oxidation of ethane to acetaldehyde
The direct conversion of low alkane-like ethane into high-value chemicals has posed a significant challenge. Herein, the authors successfully accomplish a one-step conversion of ethane to C2 oxygenates using a Rh single-atom catalyst under mild conditions.
- Bin Li
- , Jiali Mu
- & Yunjie Ding
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Article
| Open AccessSpectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation
The authors report an in situ investigation of interfacial hydrogen spillover in Pd/ZIF-8 structures with X-ray and Raman techniques. A mechanistic picture of how Pd/ZIF-8 catalyst mediate alkyne semihydrogenation to alkynes is described.
- Qiaoxi Liu
- , Wenjie Xu
- & Yujie Xiong
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Article
| Open AccessSingle-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis
In addition to maximizing atomic utilization, single-atom catalysts with defined structures can be used to investigate catalytic mechanisms and structure-activity relationships. Here, authors study a non-thermodynamically stable Pt-N2 active site for the electrochemical hydrogen evolution reaction.
- Ziqi Zhang
- , Zhe Zhang
- & Shouhua Feng
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Article
| Open AccessAsymmetric synthesis of P-stereogenic phosphindane oxides via kinetic resolution and their biological activity
P-stereogenic heterocycles are privileged chiral ligands and bioactive compounds, but the catalytic asymmetric synthesis of P-stereogenic phosphindane derivatives is challenging. Here, the authors report a catalytic kinetic resolution of phosphindole oxides via rhodium-catalyzed diastereo- and enantioselective conjugate addition to access enantiopure Pstereogenic phosphindane and phosphindole derivatives.
- Long Yin
- , Jiajia Li
- & Dong Guo
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Review Article
| Open AccessLight-driven polymer recycling to monomers and small molecules
Chemical recycling of plastic enables renewed production of pristine materials, but generally comes at a high energy cost. This review focuses on light-driven approaches for chemically recycling and upcycling plastic waste, with emphasis on reduced energy consumption and selective transformations of challenging to recycle backbone structures.
- Laura Wimberger
- , Gervase Ng
- & Cyrille Boyer
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Article
| Open AccessA restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation
Chlorine evolution reaction and deep reconstruction of catalyst are critical issues in direct seawater electrolysis. Here, the authors propose a MoO3/CoO/carbon composite material for improved selective seawater oxidation and restricted dynamic surface self-reconstruction.
- Ling Zhou
- , Daying Guo
- & Shun Wang
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Article
| Open AccessLocking the lattice oxygen in RuO2 to stabilize highly active Ru sites in acidic water oxidation
RuO2 is highly active toward the acidic electrochemical oxygen evolution reaction but exhibits instability due to lattice oxygen oxidation. Here, authors prepare an interstitial Si-decorated RuO2 catalyst with improved stability for acidic water oxidation by suppressing lattice oxygen oxidation.
- Xinyu Ping
- , Yongduo Liu
- & Zidong Wei
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Article
| Open AccessPhoto-induced intramolecular dearomative [5 + 4] cycloaddition of arenes for the construction of highly strained medium-sized-rings
Medium-sized-ring compounds are challenging synthetic targets in organic chemistry. Here the authors report an intramolecular dearomative [5 + 4] cycloaddition of naphthalene-derived vinylcyclopropanes to construct these molecules under visible-light irradiation and a proper triplet photosensitizer.
- Min Zhu
- , Yuan-Jun Gao
- & Shu-Li You
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Article
| Open AccessPulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid
Mitigating the deactivation of noble metal-based catalysts caused by self-oxidation and toxic adsorption poses a considerable challenge in organic electro-oxidation. This study addresses the issue by employing a pulsed potential electrolysis approach to selectively electrocatalyze the oxidation of glycerol to glyceric acid using a Pt-based catalyst.
- Wei Chen
- , Liang Zhang
- & Yuqin Zou
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Article
| Open AccessN-Heterocyclic carbene-catalyzed enantioselective synthesis of planar-chiral cyclophanes via dynamic kinetic resolution
Planar-chiral cyclophanes are important for drug discovery but the enantioselective synthesis of planar-chiral cyclophanes remains challenging. Here the authors describe an N-heterocyclic carbene-catalyzed asymmetric construction of planar-chiral cyclophanes.
- Jiayan Li
- , Ziyang Dong
- & Changgui Zhao
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Article
| Open AccessBubble-water/catalyst triphase interface microenvironment accelerates photocatalytic OER via optimizing semi-hydrophobic OH radical
Temperature has demonstrated the potential to regulate the photocatalytic oxygen evolution reaction (OER). This study confirms that the temperature-induced bubble-water/catalyst triphase interface microenvironment significantly enhances OER by optimizing the formation and deprotonation of semi-hydrophobic OH radicals.
- Guanhua Ren
- , Min Zhou
- & Haifeng Wang