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Conformational Sampling of the Intrinsically Disordered C-Terminal Tail of DERA Is Important for Enzyme Catalysis 10.1021/acscatal.7b04408 2018-04-06 2-Deoxyribose-5-phosphate aldolase (DERA) catalyzes the reversible conversion of acetaldehyde and glyceraldehyde-3-phosphate into deoxyribose-5-phosphate. DERA is used as a biocatalyst for the synthesis of drugs such as statins and is a promising pharmaceutic...
Highly Selective N-Monomethylanilines Synthesis From Nitroarene and Formaldehyde via Kinetically Excluding of the Thermodynamically Favorable N,N-Dimethylation Reaction 10.1021/acscatal.8b00116 2018-04-05 The synthesis of N-monomethylamine remains a challenging topic because the N,N-dimethylation reaction is thermodynamically favorable. In this work, the kinetically controlled N-monomethylamine synthesis from nitroarene and paraformaldehyde/H2 is reported to h...
Kinetic Assessment of the Simultaneous Hydrodesulfurization of Dibenzothiophene and the Hydrogenation of Diverse Polyaromatic Structures 10.1021/acscatal.8b00629 2018-04-05 The elimination of sulfur from fossil fuels via hydrodesulfurization (HDS) is paramount to produce cleaner fuels. Ultradeep HDS refers to reducing sulfur in fuels below the 10 ppm level. Nevertheless, under such conditions, dibenzothiophenes (DBTs) are to be ...
Engineering Molecular Iodine Catalysis for Alkyl–Nitrogen Bond Formation 10.1021/acscatal.8b00286 2018-04-05 An advanced protocol for the intramolecular C–H amination of alkyl groups via amidyl radicals (Hofmann–Löffler reaction) under homogeneous iodine catalysis is reported. This protocol employs common mCPBA as terminal oxidant. It proceeds under mild conditions,...
Enzyme engineering based on X-ray structures and kinetic profiling of substrate libraries: alcohol dehydrogenases for stereospecific synthesis of a broad range of chiral alcohols 10.1021/acscatal.8b00364 2018-04-04 The narrow substrate scope of naturally occurring alcohol dehydrogenases (ADHs) greatly limits the enzymatic synthesis of important chiral alcohols. Based on X-ray crystal structures and kinetic profiling of a substrate library, we engineered variants of the ...
DMF-Promoted Redox-Neutral Ni-Catalyzed Intramolecular Hydroarylation of Alkene with Simple Arene 10.1021/acscatal.8b00554 2018-04-04 A redox-neutral Ni-catalyzed intramolecular hydroarylation of alkene with simple arene has been developed, in which DMF played a proton shuttle role in facilitating the intramolecular coupling, avoiding the use of additional reductants and oxidants. A series ...
Nature of Active Nickel Sites and Initiation Mechanism for Ethylene Oligomerization on Heterogeneous Ni-beta Catalysts 10.1021/acscatal.7b03970 2018-04-04 Higher olefins produced via ethylene oligomerization are versatile commodity chemicals serving a vast range of industries with large global economic impact. Nickel aluminosilicates are promising candidates to replace the homogeneous catalysts employed in indu...
Ultrarapid in Situ Synthesis of Cu2S Nanosheet Arrays on Copper Foam with Room-Temperature-Active Iodine Plasma for Efficient and Cost-Effective Oxygen Evolution 10.1021/acscatal.8b00032 2018-04-03 Developing simple and cost-effective methods for the rapid synthesis of oxygen evolution reaction (OER) electrocatalysts from earth-abundant elements is a highly desired yet challenging task. Herein we report a two-step strategy based on the use of a room-tem...
Climbing the volcano of electrocatalytic activity while avoiding catalyst corrosion: Ni₃P, a hydrogen evolution electrocatalyst stable in both acid and alkali 10.1021/acscatal.7b04466 2018-04-03 We report microcrystalline Ni₃P as a noble-metal-free electrocatalyst for the H₂ evolution reaction (HER) with high activity just below Ni₅P₄ and Pt, the two most efficient HER catalysts known. Ni₃P has p...
Palladium Catalyzed Carbonylative Coupling of Alkyl Boron Reagents with Bromodifluoroacetamides 10.1021/acscatal.8b00420 2018-04-03 A catalytic protocol for the preparation of α,α-difluoro-β-alkyl-β-ketoamides is developed employing a Pd-mediated carbonylative Suzuki coupling between alkylboron reagents and bromodifluoroacetamides with COgen as the CO source. The reaction reveals good fun...

Conformational Sampling of the Intrinsically Disordered C-Terminal Tail of DERA Is Important for Enzyme Catalysis

10.1021/acscatal.7b04408

2018-04-06

2-Deoxyribose-5-phosphate aldolase (DERA) catalyzes the reversible conversion of acetaldehyde and glyceraldehyde-3-phosphate into deoxyribose-5-phosphate. DERA is used as a biocatalyst for the synthesis of drugs such as statins and is a promising pharmaceutic...

Highly Selective N-Monomethylanilines Synthesis From Nitroarene and Formaldehyde via Kinetically Excluding of the Thermodynamically Favorable N,N-Dimethylation Reaction

10.1021/acscatal.8b00116

2018-04-05

The synthesis of N-monomethylamine remains a challenging topic because the N,N-dimethylation reaction is thermodynamically favorable. In this work, the kinetically controlled N-monomethylamine synthesis from nitroarene and paraformaldehyde/H2 is reported to h...

Kinetic Assessment of the Simultaneous Hydrodesulfurization of Dibenzothiophene and the Hydrogenation of Diverse Polyaromatic Structures

10.1021/acscatal.8b00629

2018-04-05

The elimination of sulfur from fossil fuels via hydrodesulfurization (HDS) is paramount to produce cleaner fuels. Ultradeep HDS refers to reducing sulfur in fuels below the 10 ppm level. Nevertheless, under such conditions, dibenzothiophenes (DBTs) are to be ...

Engineering Molecular Iodine Catalysis for Alkyl–Nitrogen Bond Formation

10.1021/acscatal.8b00286

2018-04-05

An advanced protocol for the intramolecular C–H amination of alkyl groups via amidyl radicals (Hofmann–Löffler reaction) under homogeneous iodine catalysis is reported. This protocol employs common mCPBA as terminal oxidant. It proceeds under mild conditions,...

Enzyme engineering based on X-ray structures and kinetic profiling of substrate libraries: alcohol dehydrogenases for stereospecific synthesis of a broad range of chiral alcohols

10.1021/acscatal.8b00364

2018-04-04

The narrow substrate scope of naturally occurring alcohol dehydrogenases (ADHs) greatly limits the enzymatic synthesis of important chiral alcohols. Based on X-ray crystal structures and kinetic profiling of a substrate library, we engineered variants of the ...

DMF-Promoted Redox-Neutral Ni-Catalyzed Intramolecular Hydroarylation of Alkene with Simple Arene

10.1021/acscatal.8b00554

2018-04-04

A redox-neutral Ni-catalyzed intramolecular hydroarylation of alkene with simple arene has been developed, in which DMF played a proton shuttle role in facilitating the intramolecular coupling, avoiding the use of additional reductants and oxidants. A series ...

Nature of Active Nickel Sites and Initiation Mechanism for Ethylene Oligomerization on Heterogeneous Ni-beta Catalysts

10.1021/acscatal.7b03970

2018-04-04

Higher olefins produced via ethylene oligomerization are versatile commodity chemicals serving a vast range of industries with large global economic impact. Nickel aluminosilicates are promising candidates to replace the homogeneous catalysts employed in indu...

Ultrarapid in Situ Synthesis of Cu2S Nanosheet Arrays on Copper Foam with Room-Temperature-Active Iodine Plasma for Efficient and Cost-Effective Oxygen Evolution

10.1021/acscatal.8b00032

2018-04-03

Developing simple and cost-effective methods for the rapid synthesis of oxygen evolution reaction (OER) electrocatalysts from earth-abundant elements is a highly desired yet challenging task. Herein we report a two-step strategy based on the use of a room-tem...

Climbing the volcano of electrocatalytic activity while avoiding catalyst corrosion: Ni₃P, a hydrogen evolution electrocatalyst stable in both acid and alkali

10.1021/acscatal.7b04466

2018-04-03

We report microcrystalline Ni₃P as a noble-metal-free electrocatalyst for the H₂ evolution reaction (HER) with high activity just below Ni₅P₄ and Pt, the two most efficient HER catalysts known. Ni₃P has p...

Palladium Catalyzed Carbonylative Coupling of Alkyl Boron Reagents with Bromodifluoroacetamides

10.1021/acscatal.8b00420

2018-04-03

A catalytic protocol for the preparation of α,α-difluoro-β-alkyl-β-ketoamides is developed employing a Pd-mediated carbonylative Suzuki coupling between alkylboron reagents and bromodifluoroacetamides with COgen as the CO source. The reaction reveals good fun...