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Chem Catalysis
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New articles

Articles below are published ahead of final publication in an issue. Please cite articles in the following format: authors, (year), title, journal, DOI.

September 23, 2022

Review

Enabling resource circularity through thermo-catalytic and solvent-based conversion of waste plastics

  • Siddhesh S. Borkar,
  • Ryan Helmer,
  • Fatima Mahnaz,
  • Wafaa Majzoub,
  • Waad Mahmoud,
  • Ma’moun Al-Rawashdeh,
  • Manish Shetty
First published:September 23, 2022
On the path to address plastic pollution, thermochemical and catalytic processes have shown promising results for polymer recycling and upcycling. The classes of depolymerization reactions presented here have been reviewed in detail and tabulated for comparison, conveying the potential of hydroconversion and solvolysis in the transition to a circular plastics economy. The challenges deduced here portray the gaps this community needs to address to meet the broader environmental challenge.

September 22, 2022

Review

Sulfur vacancy engineering of metal sulfide photocatalysts for solar energy conversion

  • Na Zhang,
  • Zipeng Xing,
  • Zhenzi Li,
  • Wei Zhou
First published:September 22, 2022
Photocatalysis is an emerging green technology that utilizes sunlight. Metal sulfides have attracted attention in the field of photocatalysis due to their excellent properties. However, sulfides have serious photocorrosion problems. Sulfur vacancy engineering cannot only improve its optical and electrical properties but also change its surface properties. This review discusses the recent progress of metal sulfide sulfur vacancy engineering in improving photocatalytic performance and environmental remediation, as well as future development prospects and opportunities.

September 21, 2022

Article

Dynamic electrocatalysis: Examining resonant catalytic rate enhancement under oscillating electrochemical potential

  • Adam Baz,
  • Mason Lyons,
  • Adam Holewinski
First published:September 21, 2022
Certain electrocatalytic reactions can be accelerated by varying the applied potential with time. Requirements for this promotional effect are identified and contrasted with other approaches attempting to create catalysts that accelerate reaction rates with dynamically tunable surface properties.
Review

Recent advances and challenges of electrochemical ammonia synthesis

  • Xianbiao Fu,
  • Jiahao Zhang,
  • Yijin Kang
First published:September 21, 2022
Green ammonia synthesis is one of the key components to enable sustainability of new energy systems such as hydrogen economy; hence, the highly energy-consuming and carbon-emitting Haber-Bosch process using fossil fuel-derived hydrogen has to be improved or replaced if possible. Green ammonia synthesis directly from water and air is thermodynamically feasible but intangible. Li-mediated nitrogen reduction and a nitrate pathway that combines oxidative fixation and nitrate/NOx reduction might be viable candidates for a revolutionary replacement of the Haber-Bosch/Ostwald system.

September 16, 2022

Review

Enantioselective C−H functionalization reactions enabled by cobalt catalysis

  • Yang Zheng,
  • Chao Zheng,
  • Qing Gu,
  • Shu-Li You
First published:September 16, 2022
Enantioselective functionalization of C–H bonds offers a powerful solution and transformative tool for the step- and atom-economical construction of chiral molecular complexity. Recently, cobalt, as a 3d transition metal and group 9 metal, has earned considerable attention. Herein, we summarize and discuss four representative catalytic modes of cobalt catalysis, thus expecting to increase the interest of researchers in related fields and promote further developments in this area.
Perspective

Catalytic asymmetric olefin isomerization: Facile access to chiral carbon-stereogenic olefinic compounds

  • Xufang Liu,
  • Qiang Liu
First published:September 16, 2022
Catalytic asymmetric olefin isomerization is a powerful tool to access chiral carbon-stereogenic olefinic compounds, which is important for organic synthesis on the laboratory scale, as well as for large-scale industrial applications. Herein, we summarize the major developments of this field, critically discuss the plausible mechanisms, and offer our perspective of the state and challenges of this field.

September 14, 2022

Article

Pyrrolo[2,1-a]isoquinolines as multitasking organophotocatalysts in chemical synthesis

  • Yuliang Liu,
  • Haoyu Li,
  • Eugene Yew Kun Tan,
  • Erik Budi Santiko,
  • Youhei Chitose,
  • Manabu Abe,
  • Shunsuke Chiba
First published:September 14, 2022
Open Access
Chiba and co-workers have designed and developed pyrrolo[2,1-a]isoquinolines (PIqs) bearing electron-withdrawing groups as organic photocatalysts that display superior redox and energy-transfer functions to catalyze a series of molecular transformations.

September 12, 2022

Article

Modulating hydrogen bonding in single-atom catalysts to break scaling relation for oxygen evolution

  • Peiyu Ma,
  • Chen Feng,
  • Yuan Kong,
  • Dongdi Wang,
  • Ming Zuo,
  • Sicong Wang,
  • Ruyang Wang,
  • Lingling Kuang,
  • Xilan Ding,
  • Shiming Zhou,
  • Zhirong Zhang,
  • Jie Zeng,
  • Jun Bao
First published:September 12, 2022
A facile strategy for breaking the scaling relation of single-atom catalysts for oxygen evolution is proposed. Ir1/Co0.8Cu0.2OOH with cationic vacancies adjacent to the single-atom sites differentiates the similar adsorption behaviors of ∗OH and ∗OOH, circumventing their correlated free energies for a lower energy barrier at the rate-determining step, leading to a broken scaling relation.

September 8, 2022

Article

Palladium-catalyzed diastereo- and enantioselective desymmetric hydrophosphination of cyclopropenes

  • Yiliang Zhang,
  • Yanxin Jiang,
  • Mingliang Li,
  • Zhongxing Huang,
  • Jun (Joelle) Wang
First published:September 08, 2022
Transition metal-catalyzed asymmetric hydrophosphination is the most efficient and direct pathway for the synthesis of phosphine compounds. The easy accessibility and modular structure of these phosphine products afforded by this method will offer potential chiral phosphine ligands toward the study of more challenging and unprecedented reactions in asymmetric catalysis.

September 1, 2022

Review

Reticular chemistry for improving the activity of biocatalysts: Synthesis strategies and advanced characterization techniques

  • Jieying Liang,
  • Qianfan Chen,
  • Jueyi Xue,
  • Kang Liang
First published:September 01, 2022
Biocatalysis has been developed as a powerful technology for chemical innovation both in academia and across many industries. Enzymes are customized biomacromolecules that can efficiently catalyze specific conversions under defined environmental constraints. Reticular chemistry can promote and refine bioreactivity of enzymes, which is crucial to facilitate their industrial application. The continued ingenuity of materials development, as well as the growing power and complexity of protein engineering techniques, is expected to provide boundless surprises in the field of biocatalysis.
Perspective

Into the unknown: Micro/nanomotors propelled by biocatalysis based on metal-organic frameworks

  • Yu Liu,
  • Jun Ge
First published:September 01, 2022
Autonomously self-propelled items of micron to nanometer sizes that are capable of responding to signals and stimuli in the environment and reorganizing themselves to perform complex tasks are of great importance and wide interest in the fields of drug delivery, imaging, biosensing, and environmental remediation. The combination of enzyme catalysis and porous metal-organic frameworks offers a new opportunity for the development of versatile, biocompatible, fuel-bioavailable micro/nanomotors.

August 24, 2022

Review

Recent advances for the catalytic asymmetric construction of medium-sized rings

  • Ting Yao,
  • Jia Li,
  • Chengming Jiang,
  • Changgui Zhao
First published:August 24, 2022
This review provides a concise overview of the most recent breakthroughs in catalytic asymmetric synthesis of medium-sized rings. Strategies involving transition-metal catalysis and organocatalysis are discussed, with a particular interest in the proposed catalytic cycle. The aim of this review is to inspire further innovation for the asymmetric construction of medium-sized rings.

August 23, 2022

Article

The role of binding modules in enzymatic poly(ethylene terephthalate) hydrolysis at high-solids loadings

  • Rosie Graham,
  • Erika Erickson,
  • Richard K. Brizendine,
  • Davinia Salvachúa,
  • William E. Michener,
  • Yaohao Li,
  • Zhongping Tan,
  • Gregg T. Beckham,
  • John E. McGeehan,
  • Andrew R. Pickford
First published:August 23, 2022
Open Access
Enzymatic recycling of PET offers a promising solution to the global plastic problem. Research into accessory domains to enhance PET turnover has so far not been tested at high PET solids loadings. Here, we show that carbohydrate-binding domains do not offer any benefit at high PET solids loadings that are relevant to industrial-scale biorecycling.

August 15, 2022

Article

Three multi-enzyme cascade pathways for conversion of C1 to C2/C4 compounds

  • Junhui Zhou,
  • Xinyu Tian,
  • Qian Yang,
  • Zixuan Zhang,
  • Changjing Chen,
  • Ziheng Cui,
  • Yu Ji,
  • Ulrich Schwaneberg,
  • Biqiang Chen,
  • Tianwei Tan
First published:August 15, 2022
Junhui et al. successfully constructed three multi-enzyme pathways for synthesizing C2/C4 compounds (ethylene glycol, glycolic acid, and d-erythrose) from C1 compounds. Glycolic acid or d-erythrose pathways were proposed for the first time. Three new kinds of enzymes were found to catalyze intermediate glycolaldehyde to synthesize such C2/C4 compounds.
Perspective

The importance of interdiscipline in heterogeneous asymmetric catalysis

  • Huicong Dai,
  • Qihua Yang
First published:August 15, 2022
Heterogeneous asymmetric catalysis is one of the most economical and green methods for the preparation of optically active compounds, which is widely used in medicine, pesticides, and daily necessities. Despite considerable efforts in heterogeneous asymmetric catalysis, bottlenecks such as low stereoscopic and enantiomer selectivity and low catalytic activity continue to hinder its successful application in industry. To solve the current challenges, heterogeneous asymmetric catalysis urgently needs to cross disciplines with other fields and make breakthroughs in concepts and methods.
Review

Transition-metal-catalyzed enantioselective C−H silylation

  • Yicong Ge,
  • Xingfen Huang,
  • Jie Ke,
  • Chuan He
First published:August 15, 2022
Chiral organosilanes are important and valuable compounds that have found widespread applications in the field of synthetic chemistry, medicinal chemistry, and materials science. Over the past decade, transition-metal-catalyzed enantioselective C–H silylation has gradually maturated into a powerful tool for the synthesis of these silicon-containing molecules, featuring axial, helical, planar, carbon-stereogenic, or silicon-stereogenic chiralities, which has profoundly accelerated the iteration of chiral organosilicon science.

August 9, 2022

Article

Analysis of laboratory-evolved flavin-dependent halogenases affords a computational model for predicting halogenase site selectivity

  • Mary C. Andorfer,
  • Declan Evans,
  • Song Yang,
  • Cyndi Qixin He,
  • Anna M. Girlich,
  • Jaylie Vergara-Coll,
  • Narayanasami Sukumar,
  • K.N. Houk,
  • Jared C. Lewis
First published:August 09, 2022
Flavin-dependent halogenases (FDHs) can site-selectively halogenate a wide range of aromatic substrates. X-ray crystallography, site-directed mutagenesis, density functional theory, and molecular dynamics simulations were used to learn how site selectivity was previously altered through directed evolution. A predictive computational model for site selectivity of FDHs is presented.
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