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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 ***,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

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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 ***,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

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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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Novel fusiform core-shell-MOF derived in tact metal@carb on composite:An efficient cathode catalyst for aqueous and solid-state Zn-air batteries

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Journal of Energy Chemistry 2022年第1期31卷 385-394,I0011页

作者： Di Zhou Hongquan Fu Jilan Long kui shen Xinglong Gou Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637000SichuanChina Key Laboratory of Fuel Cell Technology of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640GuangdongChina

Owing to the varied mechanisms of ORR/OER,exploiting cost-effective bifunctional catalysts with robust ORR/OER activities and excellent performances in Zn-air batteries is still a *** this work,the Co/CoO@NSC bifunctional catalyst is obtained by using Zn-MOF@Co-MOF as *** Co/CoO@NSC composite has interconnected porous architecture with in tact metal@carb on structure,exhibiting superior electrocatalytic activities toward ORR and OER that can be comparable with the Pt/C and RuO_(2) catalysts,*** Co/CoO@NSC-based aqueous Zn-air battery achieves a high specific capacity(759.7 mAh/g)and energy density(990.5 Wh/kg),and ultra-long rechargeable property(more than 400 h/1200 cycles).The Co/CoO@NSC-based solid-state Zn-air battery also delivers an excellent performance with a long cycle life(more than 143 h/858 cycles).Most importantly,the newly synthesized and recharged Co/CoO@NSC-based solid-state Zn-air battery can be used to light up a 2 V LED lamp for more than 28 h,demonstrating the superior practicability as rechargeable power source.

关键词： Core-shell structure Metal organic framework Aqueous Zn-air battery Solid-state Zn-air battery Ultra long cycle life

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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 ***,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

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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 ***,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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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

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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 *** 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

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Effect of NH_4^+-N/NO_3^--N Ratios on Growth and Some Physiological Parameters of Chinese Cabbage Cultivars

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Pedosphere 2005年第3期15卷 310-318页

作者： CHENWei LUOJin-kui shenQi-Rong CollegeofResourceandEnvironmentalSciences NanjingAgriculturalUniversityNanjing210095（China）

The responses of three cultivars of Chinese cabbage (Brassica chmensis L.), one of the main vegetable crops in China, to different ratios of NH4+-N/NO3--N was investigated to find the optimal ratio of ammonium to nitrate for maximal growth and to explore ways of decreasing the nitrate content, increasing nitrogen use efficiency of Chinese cabbage, and determining distributions of nitrogen and carbon. Three cultivars of Chinese cabbage were hydroponically grown with three different NH4+-N/NO3--N ratios (0:10…

关键词： BEAN PHASEOLUS-VULGARIS NITRATE ACCUMULATION NITROGEN FORM MAIZE AMMONIUM EXPRESSION TRANSPORT NUTRITION CARBON ROOTS

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Effects of annealing condition and Al content on novel Fe_(73.5)Si_(13.5)B_9Cu_1Nb_(3-x)Al_x alloys

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Rare Metals 2008年第5期27卷 545-549页

作者： LIU Haishun DU Youwei MIAO Xiexing HAN kui shen Xiaopeng BU Wankui School of Sciences China University of Mining ＆ Technology Xuzhou 221008 China National Key Laboratory of Solid State Microstructure Nanjing University Nanjing 210093 China

The annealing condition, AI content, and field amplitude dependences of the complex permeability for Nb-poor Finemet type alloys, Fe73.5Si13.5B9Cu1Nba-xAlx （x = 0, 0.5, 1.5, 2.0, and 3.0）, were investigated using an impedance analyzer and X-ray diffraction. The results show that different AI contents lead to different optimum annealing conditions, and the A1 content exerts a distinct effect on microstructure thus resulting in a variety of real permeability value. For the samples annealed at 793 K for 0.5 h, the real permeability increases with an increase in A1 content when the AI content is below 2.0 at.%; as for those annealed at 793 K for 1 h and at 813 K for 0.5 h, an overall increase in real permeability can be obtained compared to those annealed at 793 K for 0.5 h. The permeability under different field amplitudes is also studied and it is found that the relaxation frequency in the lower frequency region tends to moving toward a higher frequency with an increase in field amplitude. All these might be because of the role of Nb in the annealing process and the solubility of AI in the amorphous matrix and nanocrystallized crystallites.

关键词： magnetism magnetic property impedance analysis Fe-based alloys

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