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Highly selective electrosynthesis of 3,4-dihydroisoquinoline accompanied with hydrogen production over three-dimensional hollow CoNi-based microarray electrocatalysts

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Nano Research 2024年第4期17卷 2509-2519页

作者： Yu Xin liyu chen Yingwei Li Kui Shen Guangdong Provincial Key Lab for Green Chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Electrocatalytic oxidation reaction of biomass-based derivatives is an excellent candidate to replace water oxidation for obtaining both value-added products and hydrogen(H_(2)),but the exploration of competent electrocatalysts is still highly challenging.Herein,two new types of three-dimensional self-supported hollow microarrays containing CoNi layered double hydroxide(CoNi-LDH)and N-doped carbon nanosheets decorated with CoNi alloyed nanoparticles(CoNi-NC)on carbon cloth(CC)are prepared,which are further used as efficient electrocatalysts for tetrahydroisoquinoline(THIQ)electrooxidation and hydrogen evolution reaction(HER),respectively.We demonstrate that the Co-modulated electronic environment for Ni(II)/Ni(Ⅲ)redox-looping in CoNi-LDH is the main factor to boost the selectivity of 3,4-dihydroisoquinoline(DHIQ)for the indirect electrooxidation process of THIQ.Density functional theory(DFT)calculations reveal that the Ni(Ⅲ)/Co(Ⅲ)dual sites of CoNi-LDH exhibit enhanced adsorption for THIQ but poorer adsorption for DHIQ compared to pure Co(Ⅲ)or Ni(Ⅲ).Therefore,the Ni(Ⅲ)/Co(Ⅲ)dual sites can effectively inhibit the peroxidation of DHIQ to isoquinoline(IQ)over CoNi-LDH,thus improving the selectivity of DHIQ to nearly 100%,much higher than that of its pure Ni counterpart.Moreover,CC@CoNi-NC can deliver high HER activity with low overpotential(40 mV@10 mA·cm^(-2))and high exchange current density(3.08 mA·cm^(-2)).Impressively,the assembled flow-cell device with CC@CoNi-LDH anode and CC@CoNi-NC cathode only requires low cell voltage and electricity consumption of 1.6 V and 3.50 kWh per cubic meter of H_(2)(@25 mA·cm^(-2)).

关键词： highly selective electrosynthesis dihydroisoquinolines hydrogen evolution reaction metal-organic frameworks hollow microarrays

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J-family genes redundantly regulate flowering time and increase yield in soybean

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The Crop Journal 2024年第3期12卷 944-949页

作者： Haiyang Li Zheng chen Fan Wang Hongli Xiang Shuangrong Liu Chuanjie Gou Chao Fang liyu chen Tiantian Bu Fanjiang Kong Xiaohui Zhao Baohui Liu Xiaoya Lin Guangdong Key Laboratory of Plant Adaptation and Molecular Design/Guangzhou Key Laboratory of Crop Gene Editing/Innovative Center of Molecular Genetics and Evolution School of Life SciencesGuangzhou UniversityGuangzhou 510006GuangdongChina

Soybean(Glycine max)is a short-day crop whose flowering time is regulated by photoperiod.The longjuvenile trait extends its vegetative phase and increases yield under short-day conditions.Natural variation in J,the major locus controlling this trait,modulates flowering time.We report that the three J-family genes influence soybean flowering time,with the triple mutant Guangzhou Mammoth-2 flowering late under short days by inhibiting transcription of E1-family genes.J-family genes offer promising allelic combinations for breeding.

关键词： Soybean Flowering time Yield J-family genes

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Porous framework materials for energy&environment relevant applications:A systematic review

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Green Energy & Environment 2024年第2期9卷 217-310页

作者： Yutao Liu liyu chen Lifeng Yang Tianhao Lan Hui Wang chenghong Hu Xue Han Qixing Liu Jianfa chen Zeming Feng Xili Cui Qianrong Fang Hailong Wang Libo Li Yingwei Li Huabin Xing Sihai Yang Dan Zhao Jinping Li College of Chemical Engineering and Technology Shanxi Key Laboratory of Gas Energy Efficient and Clean UtilizationTaiyuan University of TechnologyTaiyuan030024China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou510640China Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China Department of Chemistry The University of ManchesterManchesterM139PLUK Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore ZJU-Hangzhou Global Scientific and Technological Innovation Center Hangzhou311215China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun130012China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijing100083China

Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.

关键词： Porous framework materials Catalysis Separation Gas storage Carbon neutrality

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N-doped nanocarbon embedded in hierarchically porous metal-organic frameworks for highly efficient CO_(2) fixation

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Science China Chemistry 2022年第7期65卷 1411-1419页

作者： Fengfeng chen Kui Shen liyu chen Yingwei Li Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

The rational integration of multi-functional components with metal–organic frameworks(MOFs) to form MOF-based catalysts can often afford enhanced catalytic activity for specific reactions. Herein, we propose a novel strategy for the synthesis of hierarchically porous MOFs(e.g., MIL-101)-encapsulated N-doped nanocarbon(CN@MIL) by controlled pyrolysis of ionic liquids@MIL-101 precursors(ILs@MIL). The obtained CN@MIL composites not only possess abundant enlarged mesopores,but also show multi-active sites without the sacrifice of their structure stability. The CN@MIL can efficiently facilitate the mass transfer of substrates, exhibiting excellent catalytic performance in the synthesis of cyclic carbonates from epoxides and CO_(2) under mild and co-catalyst-free conditions(i.e., 90 ℃ and ambient pressure of CO_(2)). Furthermore, the multi-active Lewis acid sites and nucleophilic sites(Br ions) as well as the strong affinity of catalysts toward CO_(2)also contribute to the excellent catalytic activity of the CN@MIL. This study might open a new avenue for the rational design of MOF-based composites by employing ILs@MOF as precursors for advanced heterogeneous catalysis.

关键词： metal-organic frameworks N-doped nanocarbons encapsulation hierarchical porosity CO_(2)fixation

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Scalable synthesis of multi-shelled hollow N-doped carbon nanosheet arrays with confined Co/CoP heterostructures from MOFs for pH-universal hydrogen evolution reaction

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Science China Chemistry 2022年第3期65卷 619-629页

作者： Zhiqiao Wang Kui Shen liyu chen Yingwei Li Key Laboratory of Fuel Cell Technology of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Developing low-cost but efficient hydrogen evolution reaction(HER)electrocatalysts over whole pH values is a significant but daunting task for the large-scale application of electrochemical hydrogen production.Herein,we develop,for the first time,a scalable MOF-assisted strategy for the fabrication and microstructural optimization of multi-shelled hollow N-doped carbon nanosheet arrays with confined Co/CoP heterostructures on carbon cloth(Co/CoP@NC/CC)for boosting HER performances.The key to this strategy is the step-by-step epitaxial growth of unprecedented multilayer ZIF-L arrays on carbon cloth,which are subsequently pyrolyzed and controllably phosphorized to achieve the precise control over the shell number and nanoarchitectures of the Co/CoP@NC/CC.Impressively,the HER performances can be significantly enhanced by increasing hollow shell number,and the optimal triple-shelled hollow Co/CoP@NC/CC exhibits low overpotentials of 86,78 and 145 mV in acidic,alkaline and neutral media to deliver a current density of 10 mA cm^(-2),respectively,ranking as one of the best Co-based HER electrocatalysts over whole pH values.Further DFT calculations suggest that the Co/CoP heterostructures can effectively boost the cleavage of H–OH to generate protons and optimize the adsorption energy of hydrogen(ΔG_(H*)),which,together with the large electrode/electrolyte interface and accelerated charge/mass transfer of multi-shelled hollow array structure as well as the good conductivity and dispersity,are responsible for the remarkably improved HER performances.This study not only provides a new toolbox for enriching the family of multi-shelled nanoarchitecture materials,but also points out a general and effective route to develop highly efficient self-supported electrode materials for energy-related applications and beyond.

关键词： multi-shelled hollow arrays metal-organic frameworks multilayer ZIF-L arrays Co/CoP heterostructures hydrogen evolution reaction

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Corrigendum to“GmTOC1b negatively regulates resistance to Soybean mosaic virus”.[Crop J.11(2023)1762-1773]

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The Crop Journal 2024年第1期12卷 320-320页

作者： Yuhang Zhang Haiping Du Tiantian Zhao Chunmei Liao Tu Feng Jun Qin Baohui Liu Fanjiang Kong Zhijun Che liyu chen Guangdong Key Laboratory of Plant Adaptation and Molecular Design Guangzhou Key Laboratory of Crop Gene EditingInnovative Center of Molecular Genetics and EvolutionSchool of Life SciencesGuangzhou UniversityGuangzhou 510006GuangdongChina Hebei Laboratory of Crop Genetics and Breeding National Soybean Improvement Center Shijiazhuang Sub-CenterHuang-Huai-Hai Key Laboratory of Biology and Genetic Improvement of SoybeanMinistry of Agriculture and Rural AffairsInstitute of Cereal and Oil CropsHebei Academy of Agricultural and Forestry SciencesShijiazhuang 050035HebeiChina School of Ecological Engineering Guizhou University of Engineering ScienceBijie 551700GuizhouChina School of Agriculture Ningxia UniversityYinchuan 750021NingxiaChina College of Life Science Hebei Normal UniversityShijiazhuang 050024HebeiChina

The authors regret to report a mistake in the text and an associated change necessary to section 3.6 of the paper.On page 1766 in the right-hand column,line 4,the heading of subsection 3.6“GmWRKY40 represses the expression of PR genes”should be changed to“GmWRKY40 promotes the expression of PR genes”.The authors would like to apologize for any inconvenience caused.

关键词： Cor heading resistance

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Carbon-based nanoarrays embedded with Ce-doped ultrasmall Co_(2)P nanoparticles enable efficient electrooxidation of 5-hydroxymethylfurfural coupled with hydrogen production

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Science China Chemistry 2023年第7期66卷 2141-2152页

作者： Shangfang Xie Hongchuan Fu liyu chen Yingwei Li Kui Shen Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

The electrooxidation of 5-hydroxymethylfurfural(HMFOR)not only offers a green route to attain high-value 2,5-furandicarboxylic acid(FDCA)from biomass,but also is considered as a promising approach to replace the kinetically sluggish OER for future hydrogen production.Herein,we report the construction and structural optimization of Ce-doped ultrasmall Co_(2)P nanoparticles(NPs)in carbon-based nanoarrays to boost HER-coupled HMFOR.We demonstrate that the electronic structure of Co-based electrocatalysts can be positively regulated by Ce doping and the optimized Ce-Co_(2)P-based electrocatalyst only require a low voltage of 1.20 V vs.RHE to achieve 10 m A cm^(-2)for HMFOR with an excellent FDCA Faraday efficiency(FEFDCA)of 98.5%,which are superior to its Ce-free counterpart(1.29 V vs.RHE;FEFDCA=83.9%).When being assembled into a HERcoupled HMFOR system,this bifunctional electrocatalyst can achieve 50 m A cm^(-2)with an ultralow voltage of 1.46 V,which is reduced by 210 m Vas compared with that of its Ce-free counterpart(1.67 V).Quasi-operando experiments and DFTcalculations further reveal the significant roles of Ce doping in promoting the charge transfer between active sites and HMF,and reducing the free energy barrier of intermediate(^(*)HMFCA)dehydrogenation.This study provides new insights into the underlying mechanisms of Ce doping into metal phosphides for boosting HER-coupled HMFOR,developing a facile methodology to construct efficient electrocatalysts for energy storage/conversion systems.

关键词： ultrasmall Co_(2)P nanoparticles Ce doping nanosheet arrays 5-hydroxymethylfurfural electrooxidation hydrogen evolution reaction

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Facet-selective growth of MOF-on-MOF heterostructures enables etching-free synthesis of highly-open Co/N-doped carbon nanoframes for efficient catalysis

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Science China Chemistry 2022年第12期65卷 2450-2461页

作者： Yaohui Wu liyu chen Xianfeng Yang Yingwei Li Kui Shen Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou510640China State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou510640China Analytical and Testing Centre South China University of TechnologyGuangzhou510640China

Highly-open nanoframe structures consisting of interconnected and exposed ridges are highly desirable for achieving efficient catalysis,but preparing them by a facile etching-free methodology is still a very daunting task.Herein,we propose a novel metal-organic framework(MOF)-assisted and etching-free strategy for the construction of Co/N-doped carbon nanoframes with highly-open and precisely-controllable structures.This strategy is based on the face-selective epitaxial growth of ZIF-67 on the 36{110}facets of 72-facet ZIF-8 to form an unprecedented anisotropic ZIF-67-on-ZIF-8 heterostructure,which is subsequently pyrolyzed under Ar atmosphere to realize a solid-to-frame transformation.The highly-open nanoframe structure enables the substrates to readily penetrate into the catalyst interior and thereby create additional exposed active sites,which together with the good mass transport,high atomic utilization and increased surface area are responsible for its remarkably enhanced catalytic activity for the biomass valorisation when compared with its solid and closed hollow counterparts.This study could shed valuable insights into the design and preparation of various highly-open nanoframes with abundant exposed active species by using an etching-free strategy for efficient catalysis and beyond.

关键词： metal-organic frameworks etching-free synthesis highly-open nanoframes pyrolysis efficient catalysis

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A Janus heteroatom-doped carbon electrocatalyst for hydrazine oxidation

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National Science Review 2023年第3期10卷 152-162页

作者： Jieting Ding Hao-Fan Wang Xianfeng Yang Wenbo Ju Kui Shen liyu chen Yingwei Li School of Chemistry and Chemical Engineering South China University of Technology Analytical and Testing Centre South China University of Technology School of Physics and Optoelectronics South China University of Technology

The trade-off between the intrinsic activity and electronic conductivity of carbon materials is a major barrier for electrocatalysis.We report a Janus-type carbon material combining electrically conductive nitrogen-doped carbon(NC) and catalytically active boron,nitrogen co-doped carbon(BNC).The integration of NC with BNC can not only ensure high electronic conductivity of the hybrid,but also achieve an enhancement in the intrinsic activity of the BNC side due to the electron redistribution on their coupling interfaces.In the electro catalytic hydrazine oxidation reaction(HzOR),the Janus carbon electrocatalyst exhibits superior activity than their single counterparts and simple physical mixtures.D ensity functional theory calculations reve al that the NC/BNC interfaces simultaneously promote efficient electron transport and decrease the free energy of the rate-determining step in the HzOR process.

关键词： electronic conductivity heteroatom-doped carbon hydrazine oxidation reaction intrinsic activity metal–organic frameworks

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Resisting metal aggregation in pyrolysis of MOFs towards highdensity metal nanocatalysts for efficient hydrazine assisted hydrogen production

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Nano Research 2023年第5期16卷 6067-6075页

作者： Jieting Ding Danyu Guo Anqian Hu Xianfeng Yang Kui Shen liyu chen Yingwei Li School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640China Analytical and Testing Centre South China University of TechnologyGuangzhou 510640China South China University of Technology-Zhuhai Institute of Modern Industrial Innovation Zhuhai 519175China

The preparation of supported high-density metal nanoparticles(NPs)is of great importance to boost the performance in heterogeneous catalysis.Thermal transformation of metal-organic frameworks(MOFs)has been demonstrated as a promising route for the synthesis of supported metal NPs with high metal loadings,but it is challenge to achieve uniform metal dispersion.Here we report a strategy of“spatial isolation and dopant anchoring”to resist metal aggregation in the pyrolysis of MOFs through converting a bulk MOF into dual-heteroatom-containing flower-like MOF sheets(B/N-MOF-S).This approach can spatially isolate metal ions and increase the number of anchoring sites,thus efficiently building physical and/or chemical barriers to cooperatively prevent metal NPs from aggregation in the high-temperature transformation process.After thermolysis at 1,000℃,the B/N-MOFS affords B,N co-doped carbon-supported Co NPs(Co/BNC)with uniform dispersion and a high Co loading of 37.3 wt.%,while untreated bulk MOFs yield much larger sizes and uneven distribution of Co NPs.The as-obtained Co/BNC exhibits excellent electrocatalytic activities in both hydrogen evolution and hydrazine oxidation reactions,only a voltage of 0.617 V at a high current density of 100 mA·cm^(−2)is required when applied to a two-electrode overall hydrazine splitting electrolyzer.

关键词： electrocatalysis metal-organic frameworks metal nanoparticles overall hydrazine splitting thermal transformation

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