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Engineering crop nutrient efficiency for sustainable agriculture

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Journal of Integrative Plant Biology 2017年第10期59卷 710-735页

作者： liyu chen Hong Liao State Key Laboratory for Conservation and Utilization of Subtropical Agro-bioresources South China Agricultural University Guangzhou510642 China Root Biology Center Fujian Agriculture and Forestry University Fuzhou 350002 China

Increasing crop yields can provide food,animal feed, bioenergy feedstocks and biomaterials to meet increasing global demand; however, the methods used to increase yield can negatively affect sustainability. For example, application of excess fertilizer can generate and maintain high yields but also increases input costs and contributes to environmental damage through eutrophication, soil acidification and air pollution. Improving crop nutrient efficiency can improve agricultural sustainability by increasing yield while decreasing input costs and harmful environmental effects. Here, we review the mechanisms of nutrient efficiency(primarily for nitrogen, phosphorus, potassium and iron) and breeding strategies for improving this trait, along with the role of regulation of gene expression in enhancing crop nutrient efficiency to increase yields. We focus on the importance of root system architecture to improve nutrient acquisition efficiency, as well as the contributions of mineral translocation, remobilization and metabolic efficiency to nutrient utilization efficiency.

关键词： Engineering crop nutrient efficiency for sustainable agriculture

Quasi-MOF-immobilized metal nanoparticles for synergistic catalysis

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Science China Chemistry 2020年第11期63卷 1601-1607页

作者： liyu chen Nobuko Tsumori Qiang Xu AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory(ChEM-OIL) National Institute of Advanced Industrial Science and Technology(AIST)YoshidaSakyo-kuKyoto 606-8501Japan Toyama National College of Technology 13 Hongo-machiToyama 939-8630Japan School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Through partial deligandation of metal-organic frameworks(MOFs),quasi-MOFs with a transition structure between MOFs and metal compounds(such as metal oxides,nitrides,sulfides,and phosphides)can be ***-MOFs can not only retain the porous structure of MOFs to a certain extent,but also expose the inorganic nodes to the guest species(e.g.,metal nanoparticles)to show enhanced metal-support interaction for synergistic *** concept was first demonstrated by our group through calcining Au/MIL-101 at different temperatures under Ar flow to adjust the interface between Au nanoparticles and the inorganic Cr–O *** obtained Au/quasi-MIL-101 showed superior enhanced catalytic activity in the oxidation of carbon *** study has inspired further research interest to fabricate other quasi-MOFs through controlled deligandation of mono-and bimetallic MOFs and their composites for the design of efficient catalysts.

关键词： MOFs metal nanoparticles metal-support interaction quasi-MOFs synergistic catalysis

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 ***,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 *** 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/***,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 *** 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 *** 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

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 ***,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),*** 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 *** 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 ***,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

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 ***,we report the construction and structural optimization of Ce-doped ultrasmall Co_(2)P nanoparticles(NPs)in carbon-based nanoarrays to boost HER-coupled *** 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 *** 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 ***;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)*** 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

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 ***,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 *** 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 *** 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 *** 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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Encapsulation of ultrafine Pd nanoparticles within the shallow layers of UiO-67 for highly efficient hydrogenation reactions

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Science China Chemistry 2021年第1期64卷 109-115页

作者： Zhiming Cui Ting Fan liyu chen Ruiqi Fang Chuanmao Li Yingwei Li State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China Guangzhou Keneng Cosmetics Scientific Research Co. Lid.Guangzhou 510800China

Metal-organic frameworks(MOFs)have been used to encapsulate active metal nanoparticles(MNPs)to fabricate MNPs@MOFs composites with high catalytic ***,the diffusion of reactants and the accessibility of MNPs located in the center of MOFs may be hindered due to the inherent microporous structures of MOFs,which would affect the catalytic activities of ***,we report a solvent assisted ligand exchange-hydrogen reduction(SALE-HR)strategy to selectively encapsulate ultrafine MNPs(Pd or Pt)within the shallow layers of a MOF,i.e.,*** particle sizes of the encapsulated MNPs and the thickness of the MNPs-embedded layers can be adjusted easily by controlling the SALE conditions(*** and temperature).Crucially,the LE-Pd@UiO-80-0.5 composite with the thinnest Pd-embedded layers displays remarkable catalytic efficiency with a high turnover frequency(TOF)value of 600 h^-1towards hydrogenation of nitrobenzene under 1 atm H_2at room *** results indicate that the catalytic efficiency and the utilization of MNPs can be enhanced by compactly encapsulating MNPs within the shallow layers of MOFs as close to their outer surfaces as possible,owing to the short masstransfer distance and enhanced accessibility of overall MNPs.

关键词： Metal-organic frameworks metal nanoparticles heterogeneous catalysis encapsulation hydrogenation

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 *** 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 *** 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 *** 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 *** 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

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 *** 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 *** 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