Transformation of CO and H to C chemicals and fuels.

This perspective highlights the progress of CO hydrogenation to multicarbon (C) products, by discussing some typical related works, future opportunities and challenges.

Synergy of Cu/C N Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid.

Electrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g-C N ) supported Cu nanoparticles (Cu-CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm in CORR.

Oxidation of metallic Cu by supercritical CO and control synthesis of amorphous nano-metal catalysts for CO electroreduction.

Amorphous nano-metal catalysts often exhibit appealing catalytic properties, because the intrinsic linear scaling relationship can be broken. However, accurate control synthesis of amorphous nano-metal catalysts with desired size and morphology is a challenge. In this work, we discover that Cu(0) could be oxidized to amorphous CuO species by supercritical CO.

Enhanced Room Temperature Ferromagnetism in Highly Strained 2D Semiconductor CrGeTe.

Emergent magnetism in van der Waals materials offers exciting opportunities in fabricating atomically thin spintronic devices. One pertinent obstacle has been the low transition temperatures () inherent to these materials, precluding room temperature applications. Here, we show that large structural gradients found in highly strained nanoscale wrinkles in CrGeTe (CGT) lead to significant increases of .

Enhancing CO electroreduction to CH over Cu nanoparticles supported on N-doped carbon.

The electroreduction of CO to CH has attracted extensive attention. However, it is still a challenge to achieve high current density and faradaic efficiency (FE) for producing CH because the reaction involves eight electrons and four protons. In this work, we designed Cu nanoparticles supported on N-doped carbon (Cu-np/NC).

Co(NO)/covalent organic framework nanoparticles for high-efficiency photocatalytic oxidation of thioanisole.

Herein, we demonstrated a highly efficient photocatalytic sulfide oxidation reaction at ambient conditions without a sacrificial reagent or redox mediator, by using Co(NO)/covalent organic framework nanoparticles as a photocatalyst.

The study of surface species and structures of oxide-derived copper catalysts for electrochemical CO reduction.

Oxide-derived copper (OD-Cu) has been discovered to be an effective catalyst for the electroreduction of CO to C2+ products. The structure of OD-Cu and its surface species during the reaction process are interesting topics, which have not yet been clearly discussed. Herein, surface-enhanced Raman spectroscopy (SERS), operando X-ray absorption spectroscopy (XAS), and O isotope labeling experiments were employed to investigate the surface species and structures of OD-Cu catalysts during CO electroreduction.

Boosting the Productivity of Electrochemical CO Reduction to Multi-Carbon Products by Enhancing CO Diffusion through a Porous Organic Cage.

Electroreduction of CO into valuable fuels and feedstocks offers a promising way for CO utilization. However, the commercialization is limited by the low productivity. Here, we report a strategy to enhance the productivity of CO electroreduction by improving diffusion of CO to the surface of catalysts using porous organic cages (POCs) as an additive.

Efficient synthesis of cyclic carbonates from CO under ambient conditions over Zn(betaine)Br: experimental and theoretical studies.

It is very interesting to synthesize high value-added chemicals from CO under mild conditions with low energy consumption. Here, we report that a novel catalyst, Zn(betaine)Br, can efficiently promote the cycloaddition of CO with epoxides to synthesize cyclic carbonates under ambient conditions (30 °C, 1 atm). DFT calculations provide important insights into the mechanism, particularly the unusual synergistic catalytic action of Zn, Br and NR, which is the critical factor for the outstanding performance of Zn(betaine)Br.

Imaging biological samples by integrated differential phase contrast (iDPC) STEM technique.

Scanning transmission electron microscopy (STEM) is a powerful imaging technique and has been widely used in current material science research. The attempts of applying STEM (annual dark field (ADF)-STEM or annular bright field (ABF)-STEM) into biological research have been going on for decades while applications have still been limited because of the existing bottlenecks in dose efficiency and non-linearity in contrast. Recently, integrated differential phase contrast (iDPC) STEM technique emerged and achieved a linear phase contrast imaging condition, while resolving signals of light elements next to heavy ones even at low electron dose.

A cryo-electron microscopy support film formed by 2D crystals of hydrophobin HFBI.

Cryo-electron microscopy (cryo-EM) has become a powerful tool to resolve high-resolution structures of biomacromolecules in solution. However, air-water interface induced preferred orientations, dissociation or denaturation of biomacromolecules during cryo-vitrification remains a limiting factor for many specimens. To solve this bottleneck, we developed a cryo-EM support film using 2D crystals of hydrophobin HFBI.

Highly Efficient CO Electroreduction to Methanol through Atomically Dispersed Sn Coupled with Defective CuO Catalysts.

Using renewable electricity to drive CO electroreduction is an attractive way to achieve carbon-neutral energy cycle and produce value-added chemicals and fuels. As an important platform molecule and clean fuel, methanol requires 6-electron transfer in the process of CO reduction. Currently, CO electroreduction to methanol suffers from poor efficiency and low selectivity.

Boosting CO Electroreduction over a Cadmium Single-Atom Catalyst by Tuning of the Axial Coordination Structure.

Guided by first-principles calculations, it was found that Cd single-atom catalysts (SACs) have excellent performance in activating CO , and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN S moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO electroreduction to CO.

Efficient propagation of the hierarchical equations of motion using the Tucker and hierarchical Tucker tensors.

We develop new methods to efficiently propagate the hierarchical equations of motion (HEOM) by using the Tucker and hierarchical Tucker (HT) tensors to represent the reduced density operator and auxiliary density operators. We first show that by employing the split operator method, the specific structure of the HEOM allows a simple propagation scheme using the Tucker tensor. When the number of effective modes in the HEOM increases and the Tucker representation becomes intractable, the split operator method is extended to the binary tree structure of the HT representation.

VHUT-cryo-FIB, a method to fabricate frozen hydrated lamellae from tissue specimens for in situ cryo-electron tomography.

Cryo-electron tomography (cryo-ET) provides a promising approach to study intact structures of macromolecules in situ, but the efficient preparation of high-quality cryosections represents a bottleneck. Although cryo-focused ion beam (cryo-FIB) milling has emerged for large and flat cryo-lamella preparation, its application to tissue specimens remains challenging. Here, we report an integrated workflow, VHUT-cryo-FIB, for efficiently preparing frozen hydrated tissue lamella that can be readily used in subsequent cryo-ET studies.

Robust selenium-doped carbon nitride nanotubes for selective electrocatalytic oxidation of furan compounds to maleic acid.

Selective oxidation of biomass-derived furan compounds to maleic acid (MA), an important bulk chemical, is a very attractive strategy for biomass transformation. However, achieving a high MA selectivity remains a great challenge. Herein, we for the first time successfully designed and fabricated Se-doped graphitic carbon nitride nanotubes with a chemical formula of CN-Se.

Efficient electroreduction of CO to C products on CeO modified CuO.

Electrocatalytic reduction of CO into multicarbon (C) products powered by renewable electricity offers one promising method for CO utilization and promotes the storage of renewable energy under an ambient environment. However, there is still a dilemma in the manufacture of valuable C products between balancing selectivity and activity. In this work, cerium oxides were combined with CuO (CeO/CuO) and showed an outstanding catalytic performance for C products.

Hydrogen-bond donor and acceptor cooperative catalysis strategy for cyclic dehydration of diols to access O-heterocycles.

Dehydrative cyclization of diols to O-heterocycles is attractive, but acid and/or metal-based catalysts are generally required. Here, we present a hydrogen-bond donor and acceptor cooperative catalysis strategy for the synthesis of O-heterocycles from diols in ionic liquids [ILs; e.g.

Understanding the Large Kinetic Isotope Effect of Hydrogen Tunneling in Condensed Phases by Using Double-Well Model Systems.

In recent years, many experiments have shown large kinetic isotope effects (KIEs) for hydrogen transfer reactions in condensed phases as evidence of strong quantum tunneling effects. Since accurate calculation of the tunneling dynamics in such systems still present significant challenges, previous studies have employed different types of approximations to estimate the tunneling effects and KIEs. In this work, by employing model systems consisting of a double-well coupled to a harmonic bath, we calculate the tunneling effects and KIEs using the numerically exact hierarchical equations of motion (HEOM) method.

Umpolung coupling of pyridine-2-carboxaldehydes and propargylic carbonates N-heterocyclic carbene/palladium synergetic catalysis.

The umpolung cross-coupling reaction of pyridine-2-carboxaldehydes and propargylic carbonates has been developed for the first time through N-heterocyclic carbene/palladium cooperative catalysis with the judicious selection of the palladium catalyst, ligand and N-heterocyclic carbene, giving the propargylic ketones regioselectively.

Manganese-Catalyzed [3 + 2] Cyclization of Ketones and Isocyanates via Inert C-H Activation.

Stoichiometric cyclomanganation of aromatic ketones and further reactions of the thus-formed manganacycles with isocyanates were first reported by Kaesz and Liebeskind in 1975 and 1990, respectively. The buildup of a closed manganese catalytic cycle for the reaction of ketones and isocyanates remains an unsolved problem. Herein, an unprecedented trio of MeZn/AlCl/AgOTf is developed to build up manganese catalysis, which enables the [3 + 2] cyclization of ketones with isocyanates via inert C-H activation to access 3-alkylidene phthalimidines in a straightforward manner unachieved by other transition metal catalyses.

Synthesis of C Chemicals from CO and H via C-C Bond Formation.

ConspectusThe severity of global warming necessitates urgent CO mitigation strategies. Notably, CO is a cheap, abundant, and renewable carbon resource, and its chemical transformation has attracted great attention from society. Because CO is in the highest oxidation state of the C atom, the hydrogenation of CO is the basic means of converting it to organic chemicals.

Molecular-scale axial localization by repetitive optical selective exposure.

We introduce an axial localization with repetitive optical selective exposure (ROSE-Z) method for super-resolution imaging. By using an asymmetric optical scheme to generate interference fringes, a <2 nm axial localization precision was achieved with only ~3,000 photons, which is an approximately sixfold improvement compared to previous astigmatism methods. Nanoscale three-dimensional and two-color imaging was demonstrated, illustrating how this method achieves superior performance and facilitates the investigation of cellular nanostructures.

Selective hydrogenation of 5-(hydroxymethyl)furfural to 5-methylfurfural over single atomic metals anchored on NbO.

5-Methylfurfural (MF) is a very useful chemical. Selective hydrogenation of biomass platform molecule 5-(hydroxymethyl)furfural (HMF) to MF using H as the reducing agent is very attractive, but challenging because hydrogenation of C=O bond in HMF is more favourable than C-OH both kinetically and thermodynamically, and this route has not been realized. In this work, we prepare isolated single atomic catalysts (SACs) Pt/NbO-Ov, Pd/NbO-Ov, and Au/NbO-Ov, in which single metal atoms are supported on oxygen defective NbO (NbO-Ov).