Xingchao Dai

Xingchao Dai
Chinese Academy of Sciences | CAS · Lanzhou Institute of Chemical Physics

Doctor of Philosophy

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49
Publications
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689
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Publications

Publications (49)
Article
Full-text available
Diminishing fossil fuel resources and calls for sustainability are driving the urgent need for efficient valorization of renewable resources with high atom efficiency. Inspired from the natural goethite mineral with Mn paragenesis, we develop cost-effective MnO 2 /goethite catalysts for the efficient valorization of dihydroxyacetone, an important b...
Article
Upgrading biomass without waste: Scientists from Rostock and Lanzhou have, for the first time, succeeded in directly converting C2−C3 biomass molecules with amines and H2O2 to industrially important formamides by valorizing all carbon atoms of the substrates without producing undesired by‐products. The reaction is catalyzed under very mild conditio...
Article
Precisely controlling the regioselectivity with monophosphine ligand is a long-standing challenge in hydroformylation. Herein, we describe the one-pot encapsulation of single-atom Rh catalysts within porous monophosphine polymers for regioselective heterogeneous hydroformylation of alkenes. The optimized catalyst ([email protected]) shows remarkabl...
Chapter
CO 2 is a cheap, abundant, renewable, and nontoxic C 1 resource, and the utilization of CO 2 as carbonyl resource for the synthesis of value‐added carbonyl compounds has attracted increasing interests from the view of environmental protection and sustainable development. The developments and recent advances in conversion of CO 2 to produce useful c...
Chapter
Non‐C 1 carbonyl molecules, including carbonyl metal, formates, formamides, formic anhydride, silacarboxylic acid, n ‐formylsaccharin, acyl chloride, and in situ generated carbonyl resource, have been developed as CO surrogates for synthesis of carbonyl compounds. In this chapter, the recent advances in carbonylation reactions using different carbo...
Chapter
Although CO has been extensively applied in chemical industry, its intrinsic properties such as high toxicity, flammability, and special equipment requirement for handling limit its utilization in organic synthesis and academia. Thus, considerable efforts have been devoted to the development of CO surrogates to avoid the direct use of CO. As cheap...
Chapter
Synthesis and transformation of carbonyl‐containing molecules constitute the core of carbonyl chemistry. These molecules can bridge the whole catalytic process and behave as reactants to provide the carbonyl sources for various carbonyl compounds (aldehydes, ketones, acids, esters, and their derivatives) synthesis; as catalysts for the acid‐catalyz...
Chapter
The transformation of carbonyl molecules is a powerful tool for the synthesis of fine and bulk chemicals as well as pharmaceuticals. Carbon monoxide (CO) represents an indispensable carbonyl reagent in the synthesis of carbonyl‐containing compounds due to its abundance, low price and high reactivity. This chapter will briefly describe the recent ad...
Chapter
Carbonyl molecules including aldehydes and ketones groups can be applied as the active species in many valuable transformations. This chapter mainly focuses on the reactions realized via carbonyl–hydroxyl groups recycling. To be specific, carbon material and related polymers containing aldehydes and ketones group as the catalyst are discussed in de...
Chapter
Carboxyl group (–CO 2 H) can be applied as the active species in many catalytic reactions. This chapter will briefly introduce the progress in the acid‐catalyzed reactions with –CO 2 H. Specifically, carboxylic acid and carboxyl functionalized carbon materials as the catalysts are discussed in this section, which presented several meaningful reacti...
Chapter
As an important class of structural motifs, carbonyl compounds display the robust synthetic utility in functional materials owing to the presence of easily transformable carbonyl group. In this chapter, synthetic applications of carbonyl compounds to produce functional materials will be discussed briefly. Particularly, the synthesis of functional m...
Chapter
Carbonyl compounds serve as key intermediates in the preparation of a variety of functional molecules. In this chapter, synthetic applications of carbonyl compounds to produce versatile chemicals will be described. Particularly, the synthesis of functional molecules is mainly focused on the transformations with carbonyl compounds as starting materi...
Article
Full-text available
The shift from fossil carbon sources to renewable ones is vital for developing sustainable chemical processes to produce valuable chemicals. In this work, value‐added formamides were synthesized in good yields by the reaction of amines with C2‐C3 biomass‐based platform molecules such as glycolic acid, 1,3‐dihydroxyacetone and glyceraldehyde. These...
Article
Based on the experimental and DFT calculation results, here for the first time we built preferential adsorption sites for nitroarenes by modification of the supported Cu catalysts surface with 1,10-phenathroline (1,10-phen), by which the yield of aniline via reduction of nitroarene is enhanced three times. Moreover, a macromolecular layer was in-si...
Article
The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO2. So far, homogeneous metal complexes have been mainly applied for such transformations. Here, we describe the synthesis of novel heterogeneous Zn-based catalysts, which were conveniently p...
Article
N-alkylamines and amides were important organic synthesis building stock and intermediates, and their synthesis has been one of the intense topics for chemists. Among the developed methods, the direct coupling of carbonyl-containing molecules such as formaldehydes, CO, and CO2 with amines and the reaction of alcohols with amines via in situ constru...
Article
of main observation and conclusion An efficient and organic ligand‐free heterogeneous catalytic system for hydroformylation of olefins is highly desirable for both academy and industry. In this study, simple Rh black was employed as a heterogeneous catalyst for hydroformylation of olefins in the absence of organic ligand. The Rh black catalyst show...
Article
For the first time, Pd supported on natural palygorskite was developed for amine formylation with CO2 and H2. Both secondary and primary amines with diverse structures could be converted into the desired formamides at < 100 °C, and good to excellent yields were obtained.
Article
A highly active Pd/TiO2 catalyst system was prepared and applied in the oxidative carbonylation of amines to ureas with ultra-low Pd content under organic ligand and solvent free conditions. The catalytic turnover frequencies (TOFs, moles of amines converted per mole of Pd per h) were 126000 and 250000 h−1 for the production of diphenylurea and dib...
Article
Full-text available
Bridging homogeneous and heterogeneous catalysis is a long-term pursuit in the field of catalysis. Herein, we report our results in integration of nano- and molecular catalysis via catalytic synthesis of nitrogen doped carbon layers on AlOx supported nano-Cu which can finely tune the catalytic performance of the supported copper catalyst. This synt...
Article
Full-text available
Nitrogen-doped carbon materials with enhanced CO2 adsorption were prepared by the salt and base co-activation method. First, resorcinol-formaldehyde resin was synthesized with a certain salt as an additive and used as a precursor. Next, the resulting precursor was mixed with KOH and subsequently carbonized under ammonia flow to finally obtain the n...
Article
Biomass‐based 1,3‐dihydroxylacetone can be converted in a sustainable one‐pot process at room temperature with 100 % atom efficiency to valuable glycolic acid, formamides, and formates. F. Shi, A. Brückner, and co‐workers showed in their Communication (DOI: 10.1002/anie.201814050), that this proceeds through a radical mechanism on a cheap catalyst,...
Article
A new and straightforward method was developed for the synthesis of N-methyl-1,2,3,4-tetrahydroquinolines by one-pot reductive N-methylation of quinolines with paraformaldehyde and H2 over Pd/C catalyst. A series of functional MTHQs,...
Article
Biomassen‐basiertes 1,3‐Dihydroxyaceton lässt sich in einem nachhaltigen Ein‐Topf‐Prozess bei Raumtemperatur mit einer Atomeffizienz von 100 % in wertvolle Glycolsäure, Formamide und Formiate überführen. F. Shi, A. Brückner et al. zeigen in ihrer Zuschrift (DOI: 10.1002/ange.201814050), dass diese Umsetzung über einen Radikalmechanismus an einem ko...
Article
Glycolic acid (GA) as important building block of biodegradable polymers has been synthesized for the first time in excellent yields at room temperature by selective oxidation of 1,3‐dihyroxyacetone (DHA) using a cheap supported Cu/Al2O3 catalyst with single active CuII species. By combining EPR spin‐trapping and operando ATR‐IR experiments, differ...
Article
Glycolic acid (GA) as important building block of biodegradable polymers has been synthesized for the first time in excellent yields at room temperature by selective oxidation of 1,3‐dihyroxyacetone (DHA) using a cheap supported Cu/Al2O3 catalyst with single active CuII species. By combining EPR spin‐trapping and operando ATR‐IR experiments, differ...
Article
N-alkyl amides have wide applications in the biological, pharmaceutical and organic chemical industry. Accordingly, its synthesis has attracted great attention. Among different methods, the N-alkylation of amides with alcohols constitutes an attractive process for their synthesis because alcohol is readily available, and water is generated as the s...
Article
Catalytic alcohol amination is a sustainable reaction for N‐alkyl amine synthesis. In the past research, homogeneous and supported copper catalysts have been extensively studied and nice resutls were obtained. In this work, we’d like to show that copper powder can behave as an active catalyst for the alcohol amination, and its catalytic performance...
Article
Here, surprising results are presented in bulk Pd catalyzed carbonylation reactions. Three types of carbonylation reactions can be realized efficiently under organic ligand-free conditions, i.e., hydroaminocarbonylation of olefins, aminocarbonylation of aryl iodides and oxidative carbonylation of amines, which almost covers all the known mechanisms...
Article
Full-text available
Generally, a homogeneous catalyst exhibits good activity and defined active sites but it is difficult to recycle. Meanwhile, a heterogeneous catalyst can easily be reused but its active site is difficult to reveal. It is interesting to bridge the gap between homogeneous and heterogeneous catalysis via controllable construction of a heterogeneous ca...
Article
Full-text available
Carbon dioxide is a green C1 resource that can be efficiently recycled by catalytic transformation into value-added chemicals. Formamides are important intermediates and solvents that are used extensively in pharmaceutical, daily-chemical, and petrochemical industry. Therefore, it is worthwhile to synthesize formamides with CO2 and amines. In this...
Article
It maintains as a challenging topic for N-monomethylamine synthesis as the N,N-dimethylation reaction is thermodynamically favorable. The kinetically controlled N-monomethylamine synthesis from nitroarene and paraformaldehyde/H2 is reported with super-high N-monomethylamine selectivity in the presence of a Pd/TiO2 catalyst. The superior selectivity...
Article
Full-text available
Catalytic hydrosilylation represents a straightforward and atom-efficient methodology for the creation of C–Si bonds. In general, the application of homogeneous platinum complexes prevails in industry and academia. Herein, we describe the first heterogeneous single atom catalysts (SACs), which are conveniently prepared by decorating alumina nanorod...
Article
The selective N-monomethylation of amines is an improtant topic in fine chemical synthesis. Herein, for the first time, we described a selective N-monomethylation reaction of amines with paraformaldehyde and H2 in the presence of CuAlOx catalyst. A variety of amines, including primary aromatic amines, benzylamine and cyclohexylamine, as well as sec...
Article
Prochiral aminoketones are key intermediates for the synthesis of optically active amino alcohols, and glycerol is one of the main biomass-based alcohols available in industry. In this work, glycerol was catalytically activated and purposefully converted with amines to generate highly valuable prochiral aminoketones, as well as N-formamides and N-m...
Article
Here, we show the results of molecular-defined conjugated ketone catalyzed alcohol amination reaction. Under the optimized reaction conditions, the yields to the desired products reached 98%. Reaction mechanism and kinetic study supposed that carbonyl-hydroxyl groups are the catalytically active sites, and the transfer-hydrogenation reactions are p...
Article
Generally, transition metal catalysts are essential for the reductive hydrogen atom transfer reaction, which is also known as the transfer hydrogenation reaction or the borrowing-hydrogen reaction. It has been reported that graphene can be an active catalyst in ethylene and nitrobenzene reductions, but no report has described carbon-based materials...
Article
Full-text available
A simple CuNiAlOx catalyst was prepared for the cooperative transformation of nitrobenzene derivatives and biomass-based alcohols. Under the optimized reaction conditions, a range of nitrobenzene derivatives can be smoothly converted into the corresponding amines and glycerol was directly transformed into 1, 3-dihydroxypropan-2-one.
Article
CO2/H-2 was successfully employed in alkylation reactions by performing CO2 reduction and amine N-methylation in one-pot. In the presence of a simple CuAlOx catalyst, N-methyl or N,N-dimethyl amines with different structures can be selectively synthesized with up to 96% yields by applying amine, nitrobenzene and nitrile as starting materials.
Article
The N-alkylation of amines or ammonia with alcohols is a valuable route for the synthesis of N-alkyl amines. However, as a potentially clean and economic choice for N-alkyl amine synthesis, non-noble metal catalysts with high activity and good selectivity are rarely reported. Normally, they are severely limited due to low activity and poor generali...
Article
An air and moisture stable heterogeneous non‐noble metal catalyst, that is NiCuFeO x, was designed and prepared for the synthesis of N‐substituted primary, secondary, tertiary, and cyclic amines by using ammonia, primary amines, or secondary amines as nitrogen sources and alcohols as alkylation reagents under base‐ and organic‐ligand‐free condition...

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