Selective electrochemical reduction of CO2 into energy-dense organic compounds is a promising strategy for using as carbon source. Herein, we investigate series iron-based catalysts synthesized by pyrolysis Fe-, N-, and C-containing precursors the electroreduction to CO under aqueous conditions demonstrate that selectivity these materials over proton governed ratio isolated FeN4 sites vs Fe-based nanoparticles. This can be synthetically tuned generate electrocatalysts producing controlled...

Abstract To use water as the source of electrons for proton or CO 2 reduction within electrocatalytic devices, catalysts are required facilitating proton‐coupled multi‐electron oxygen evolution reaction (OER, H O→O +4 + e − ). These catalysts, ideally based on cheap and earth abundant metals, have to display high activity at low overpotential good stability selectivity. While numerous examples Co, Mn, Ni were recently reported oxidation, only few using copper, despite promising efficiencies....

Significance Carbon dioxide electroreduction may constitute a key technology in coming years to valorize CO 2 as high value-added chemicals such hydrocarbons and way store intermittent solar energy durably. Based on readily available technologies, systems combining photovoltaic (PV) cell with an electrolyzer (EC) for reduction are likely strategy tackling this challenge. However, low-cost, sustainable, highly efficient PV–EC system has yet be developed. In article, we show that goal can...

Siloxides can support U! …︁in the reduction of small molecules with uranium complexes. The treatment [U{N(SiMe3)2}3] HOSi(OtBu)3 (3 equiv) yielded a novel homoleptic uranium(III) siloxide complex 1, which acted as two-electron reducing agent toward CS2 and CO2 (see scheme). Complex 1 also reduced toluene to afford diuranium inverted-sandwich complex. Detailed facts importance specialist readers are published "Supporting Information". Such documents peer-reviewed, but not copy-edited or...

Abstract To use water as the source of electrons for proton or CO 2 reduction within electrocatalytic devices, catalysts are required facilitating proton‐coupled multi‐electron oxygen evolution reaction (OER, H O→O +4 + e − ). These catalysts, ideally based on cheap and earth abundant metals, have to display high activity at low overpotential good stability selectivity. While numerous examples Co, Mn, Ni were recently reported oxidation, only few using copper, despite promising efficiencies....

Abstract Designing supported alkene metathesis catalysts with high activity and stability is still a challenge, despite significant advances in the last years. Described herein combination of strong σ‐donating N‐heterocyclic carbene ligands weak surface silanolates cationic tungsten sites leading to highly active stable catalysts. These well‐defined silica‐supported catalysts, [(≡SiO)W(=O)(=CHCMe 2 Ph)(IMes)(OTf)] Ph)(IMes) + ][B(Ar F ) 4 − ]...

Abstract Mo‐ and Fe‐containing enzymes catalyze the reduction of nitrate nitrite ions in nature. Inspired by this activity, we study here reaction (NO 3 RR) catalyzed an Fe‐substituted two‐dimensional molybdenum carbide MXene family, viz ., Mo 2 C T x : Fe ( are oxo, hydroxy fluoro surface termination groups). contains isolated sites positions host (Mo ) features a Faradaic efficiency (FE) NH yield rate 41 % 3.2 μmol h −1 mg , respectively, for NO − to 4 + acidic media 70 12.9 neutral media....

Phthalocyanines (PCs) are intriguing building blocks owing to their stability, physicochemical and catalytic properties. Although PC-based polymers have been reported before, many suffer from relatively low crystallinity, surface areas. Utilizing a mixed-metal salt ionothermal approach, we report the synthesis of series metallophthalocyanine-based covalent organic frameworks (COFs) starting 1,2,4,5-tetracyanobenzene 2,3,6,7-tetracyanoanthracene form corresponding COFs named M-pPPCs M-anPPCs,...

Useful connection: The self-assembly of four salen complexes pentavalent uranyl ions by mutual coordination affords a tetrametallic complex that is highly stable toward disproportionation and hydrolysis, shows an unambiguous antiferromagnetic coupling between the oxo-bridged uranium centers (see picture; O red, U green). first mixed-valent UV3/UVI compound has been selectively synthesized from this complex. Detailed facts importance to specialist readers are published as "Supporting...

Abstract Single‐chain magnets (SCMs) are materials composed of magnetically isolated one‐dimensional (1D) units exhibiting slow relaxation magnetization. The occurrence SCM behavior requires the fulfillment stringent conditions for exchange and anisotropy interactions. Herein, we report synthesis, structure, magnetic characterization first actinide‐containing SCM. 5f–3d heterometallic 1D chains [{[UO 2 (salen)(py)][M(py) 4 ](NO 3 )}] n , (M=Cd ( 1 ) M=Mn ); py=pyridine) assembled trough...

Grafting (ArO)2W(═O)(═CHtBu) (ArO = 2,6-mesitylphenoxide) on partially dehydroxylated silica forms mostly [(≡SiO)W(═O)(═CHtBu)(OAr)] along with minor amounts of [(≡SiO)W(═O)(CH2tBu)(OAr)2] (20%), both fully characterized by elemental analysis and IR NMR spectroscopies. The well-defined oxo alkylidene surface complex [(≡SiO)W(═O)(═CHtBu)OAr] is among the most active heterogeneous metathesis catalysts reported to date in self-metathesis cis-4-nonene ethyl oleate, sharp contrast classical based...

A broad series of fully characterized, well-defined silica-supported W metathesis catalysts with the general formula [(≡SiO)W(═NAr)(═CHCMe2R)(X)] (Ar = 2,6-iPr2C6H3 (AriPr), 2,6-Cl2C6H3 (ArCl), 2-CF3C6H4 (ArCF3), and C6F5 (ArF5); X OC(CF3)3 (OtBuF9), OCMe(CF3)2 (OtBuF6), OtBu, OSi(OtBu)3, 2,5-dimethylpyrrolyl (Me2Pyr) R Me or Ph) was prepared by grafting bis-X substituted complexes [W(NAr)(═CHCMe2R)(X)2] on silica partially dehydroxylated at 700 °C (SiO2-(700)), their activity evaluated goal...

Alkene metathesis is a widely and increasingly used reaction in academia industry because of its efficiency terms atom economy wide applicability. This notably responsible for the production several million tons propene annually. Such industrial processes rely on inexpensive silica-supported tungsten oxide catalysts, which operate at high temperatures (>350 °C), contrast with mild room temperature conditions typically corresponding molecular alkene homogeneous catalysts. large difference...

Abstract Electroreduction of CO 2 to is one the simplest ways valorise as a source carbon. Herein, cheap, robust, Cu‐based hybrid catalyst consisting polymer Cu phthalocyanine coated on carbon nanotubes, which proved be selective for production (80 % faradaic yield) at relatively low overpotentials, was developed. Polymerisation shown have drastic effect selectivity reaction because molecular instead proton reduction under same conditions. Although material only showed isolated sites in...

Terpyridine ligands are widely used in chemistry and material sciences owing to their ability form stable molecular complexes with a large variety of metal ions. In that context, variations the substituents on terpyridine ligand allow modulation properties. Applying Stille cross-coupling reaction, we prepared good yields new series possessing quinoline-type moieties ortho, meta, para positions dimethylamino at central or distal positions. The corresponding cobalt(II) were synthesized fully...

Abstract Alloying strategies are commonly used to design electrocatalysts that take on properties of their constituent elements. Herein, such a strategy is develop Zn–Cu alloyed electrodes with unique hierarchical porosity and tunable selectivity for CO 2 versus H + reduction. By varying the Zn/Cu ratio, tailored syngas mixtures obtained without production other gaseous products, which attributed preferential CO‐ ‐forming pathways alloys. The ratios also significantly less sensitive applied...