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Journal of Energy chemistry 2024年第7期94卷 778-788页

作者： Yinggang Sun Tingwei Zhang Peng Sun Jigang Wang Wenjie Duan Yanqiong Zhuang Likai Wang Zhongfang Li School of chemistry and chemical {2. Shandong University of TechnologyZibo 255049ShandongChina

The preparation of bifunctional catalysts for oxygen reduction(ORR)and oxygen evolution(OER)is crucial for Zn-air ***,we report a La doped CoFe_(2.O_(4) spinel catalyst supported on threedimensional graphene(3D-G),where La can facilitate electron transfer from Co to Fe,leading to increased electron cloud density in Fe and improved catalytic *** redshift of the G peak in the Raman spectra indicates the interaction between theπbond of 3D-G and d orbitals in La_(0.2.CoFe_(1.8)O_(4).La_(0.2.CoFe_(1.8)/3D-G exhibits superior ORR performance(E_(1/2.=0.86 V ***)and OER performance(E_(j=10)=1.55 V ***)to CoFe_(2.O_(4)/3D-G(E_(1/2.=0.831 V ***,E_(j=10)=1.603 V ***).Furthermore,it demonstrates excellent bifunctional oxygen catalytic performance while maintaining high power density and stability in liquid zinc-air batteries(ZABs)and flexible ZABs(F-ZABs).This work presents a viable strategy for utilizing rare earth element doped spinels to enhance oxygen catalyst and ZABs performance.

关键词： Zn-air batteries Electrocatalysts La_(0.2.CoFe_(1.8)/3D-G Electron pump Bifunctional oxygen catalytic performance

Cooperation between single atom catalyst and support to promote nitrogen electroreduction to ammonia:A theoretical insight

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Journal of Energy chemistry 2024年第9期96卷 336-344页

作者： Wanying Guo Siyao Wang Hongxia Wang Qinghai Cai Jingxiang Zhao College of chemistry and chemical {2. Harbin Normal UniversityHarbin 150025HeilongjiangChina

The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing multiple intermediates and ***,we utilized defective BC_(3)monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic performance of the nitrogen reduction reaction(NRR)for ammonia(NH_(3))*** results showed that these SACs can be firmly stabilized on these defective BC_(3)supports with high stability against ***,co-activation of the inert N_(2.reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N–N bond *** high-throughput screening revealed that the Mo/DV_(CC)and W/DV_(CC)exhibit superior NRR catalytic performance,characterized by a low limiting potential of−0.33 and−0.43 V,respectively,which can be further increased under acid conditions based on the constant potential ***,varying NRR catalytic activities can be attributed to the differences in the valence state of active ***,further microkinetic modeling analysis displayed that the turnover frequency of N_(2.–to–NH_(3)conversion on Mo/DV_(CC)is as large as 1.2.×10^(−3)s^(−1)site^(−1) at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction *** results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal–support interactions.

关键词： Co-catalysis Single atom catalyst Nitrogen reduction DFT computations

Chiral multiple-resonance thermally activated delayed fluorescence materials based on chiral spiro-axis skeleton for efficient circularly polarized electroluminescence

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Science China chemistry 2024年第7期67卷 2257-2264页

作者： Shi-Quan Song Xiao Han Zhong-Zhong Huo Ching-Fai Yip Xian-Fang Hong Meng-Ning Ding You-Xuan Zheng State Key Laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Key Laboratory of Mesoscopic chemistry of Ministry of Education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chiral luminescence materials have potential applications in the field of three-dimensional displays due to their circularly polarized luminescence(CPL)***,the further development of circularly polarized organic light-emitting diodes(CP-OLEDs)needs to meet the requirements of high efficiency,high color purity,low cost,and high dissymmetry factor(gPLor gEL),chiral multiple resonance thermally activated delayed fluorescence(MR-TADF)materials are considered as candidates in these ***,based on a pair of chiral spirofluorene precursors,two pairs of high-performance chiral MR-TADF emitters((R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB)are developed,which exhibit strong emissions peaking at 491 and 502.nm in toluene with full-width at half-maximum values of 2. and 33 nm,*** addition,small singlet–triplet energy gaps of 0.15 and 0.10 eV with high absolute photoluminescence efficiencies of 95.0%and 96.7%are observed for p-Spiro-DtBuCzB and m-Spiro-DtBuCzB molecules,*** based on p-Spiro-DtBuCzB and m-Spiro-DtBuCzB display high maximum external quantum efficiencies of 2..6%and 33.8%,*** importantly,CP-OLEDs present symmetric circularly polarized electroluminescence spectra with|gEL|factors of 3.36×10^(-4)and 7.66×10^(-4)for devices based on(R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB enantiomers,respectively.

关键词： chiral spiro-axis skeleton-based material multiple resonance thermally activated delayed fluorescence circularly polarized electroluminescence dissymmetry factor external quantum efficiency

Synthesis of photostable near-infrared sulfone-rhodamines for photoacoustic imaging-guided photothermal therapy

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Chinese chemical Letters 2024年第3期35卷 369-372页

作者： Huiyu Si Dongjuan Wang Xianfa Du Xin Zhou department of chemistry College of Chemistry and Chemical EngineeringQingdao UniversityQingdao 266071China department of Orthopedics the Affiliated Hospital of Qingdao UniversityQingdao 266071China

Photothermal therapy(PTT)is a cutting-edge cancer treatment that can kill cancer cells in hypoxic environments without relying on *** of the ideal photothermal agents with a high absorption coefficient in the near-infrared region,and a high excellent photothermal conversion efficiency is of great ***-Rhodanmine dye has showed an impressive absorption wavelength over 700 nm,but suffered from a stability *** this study,we synthesized five sulfone rhodamines and investigated the substitution effects on ***_(2.R2.showed high stability and strong absorbance at 714 nm with an excellent photothermal conversion efficiency of 53.06%,making it suitable for accurate photoacoustic imaging-guided photothermal therapy in vivo.

关键词： Photothermal therapy Sulfone rhodamine Near-Infrared Photoacoustic Imaging

Fully fluorinated hybrid zeolite imidazole/Prussian blue analogs with combined advantages for efficient oxygen evolution reaction

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Chinese chemical Letters 2024年第6期35卷 222-228页

作者： Jiayu Xu Meng Li Baoxia Dong Ligang Feng School of chemistry and chemical {2. Yangzhou UniversityYangzhou 225002China

Hybrid metal-organic framework(MOF)derivatives play a significant role in the novel catalyst development in energy conversion ***,we demonstrated the low-temperature fully fluorinated zeolitic imidazole framework(ZIF)coupled with a three-dimensional open framework Prussian blue analog(PBA)with combined advantages for electrocatalytic oxygen evolution reaction(OER)in water splitting *** spectroscopic analysis and the electrochemical studies revealed the combined advantages of efficient electronic effect and active site *** of good conductivity improvement by Ndoped carbon derived from ZIF and the high electrochemical surface area and active site exposure from PBA derivatives,good catalytic performance was obtained on the optimal catalyst of Co Ni ZIF/Co Fe-PBAF-300,which required a low overpotential of 2.0 m V to reach 10 m A/cm^(2.loaded on the glassy carbon electrode,with Tafel slope of 47.4 m V/dec,and very high dynamic and steady *** addition,the multi-component with the mixed structure from highly polar metal fluorides promoted the easy formation of the active phase as revealed by the post-sample *** current results showed a novel composite catalyst materials development from the hybrid MOF derivatives,which would be promising in the electrolysis of water oxidation reactions and energy-relevant catalysis reactions.

关键词： Metal-organic framework Zeolitic imidazole framework Prussian blue analog Fluoridation Multi-component Oxygen evolution reaction

Enhancing the electrocatalytic performance of nitrate reduction to ammonia by in-situ nitrogen leaching

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Chinese chemical Letters 2024年第2期35卷 564-569页

作者： Mimi Fu Yini Mao Hua Wang Wei Luo Yimin Jiang Wei Shen Ming Li Rongxing He College of chemistry and chemical {2. Southwest UniversityChongqing 400715China

Electrochemical nitrate reduction reaction (NITRR) is regarded as a “two birds-one stone” method for the treatment of nitrate contaminant in polluted water and the synthesis of valuable ammonia, which is retarded by the lack of highly reactive and selective electrocatalysts .Herein, for the first time, nickel foam supported Co_(4) N was designed as a high-performance NITRR catalyst by an in-situ nonmetal leaching-induced *** the optimal potential, the Co_(4) N/NF catalyst achieves ultra-high Faraday efficiency and NH_(3) selectivity of 95.4% and 99.4%, *** situ X-ray absorption spectroscopy (XAS), together with other experiments powerfully reveal that the nitrogen vacancies produced by nitrogen leaching are stable and play a key role in boosting nitrate reduction to *** calculations confirm that Co_(4) N with abundant nitrogen vacancies can optimize the adsorption energies of NO_(3)^(-) and intermediates, lower the free energy (Δ G ) of the potential-determining step (*NH_(3) to NH_(3) ) and inhibit the formation of N-containing *** addition, we also conclude that the nitrogen vacancies can stabilize the adsorbed hydrogen, making H_(2. quite difficult to produce, and lowering ΔG from *NO to *NOH, which facilitates the selective reduction of *** study reveals significant insights about the in-situ nonmetal leaching to enhance the NITRR activity.

关键词： Co4N Nitrate reduction In-situ nonmetal leaching Nitrogen vacancy Mechanism

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.(@2. mA·cm^(-2.).

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

Heterostructure of 2. MoSe_(2. nanosheets vertically grown on bowllike carbon for high-performance sodium storage

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Nano Research 2024年第5期17卷 4023-4030页

作者： Nianxiang Shi Guangzeng Liu Baojuan Xi Xuguang An Changhui Sun Shenglin Xiong School of chemistry and chemistry {2. Qilu Normal UniversityJinan 250200China School of chemistry and chemical {2. Shandong UniversityJinan 250100China School of Mechanical engineering Chengdu UniversityChengdu 610106China

Transition metal dichalcogenides are attractive anode materials for sodium ion batteries(SIBs)due to their high theoretical capacity and large interlayer ***,its practical application is hampered by the sluggish kinetics of Na^(+)insertion and structure collapse caused by Na^(+)insertion/***,the heterostructures of MoSe_(2. nanosheets vertically growing on bowl-like carbon(MoSe_(2.@C)are designed and prepared by a template method coupled with selenization treatment to boost storage sodium *** hollow and collapse could provide enough storage space for Na^(+)and alleviate the volume expansion during the charge/discharge ***_(2. nanosheets vertically grown on carbon could expose more active sites for adsorbing Na^(+)to enhance the utilization rate of electrode ***,building heterostructures by combining different phase components could facilitate Na^(+)diffusion and advance reaction *** from these merits,the bowl-like MoSe_(2.@C shows outstanding reversible capacity(356.8 mAh·g^(-1) after 1500 cycles at 1 A·g^(-1))and remarkable rate performance(2.9.9 mAh·g^(-1)10 A·g^(-1)).

关键词： MoSe_(2.nanosheets bowl-like carbon heterostructure sodium ion batteries

SO_(2.-Insertion induced enantioselective oxysulfonylation to access β-chiral sulfones with quaternary carbon stereocenters

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Science China chemistry 2024年第3期67卷 908-913页

作者： Jun Zhang Xuefeng Wang Peiqi Wang Jiayuan Fang Shaoyu Li Jie Wu School of Pharmaceutical and chemical engineering&Institute for Advanced Studies Taizhou UniversityShanghai 200438China department of chemistry Fudan UniversityShanghai 200438China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of chemistry and chemical {2. Henan Normal UniversityXinxiang 453007China

β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid growth of sulfur dioxide insertion chemistry over the last decade, enantioselective catalytic variants for accessing β-chiral sulfones, especially those bearing a quaternary carbon stereocenter, remain rare. Herein, we report an enantioselective copper/bisoxazoline catalyzed oxysulfonylation of alkenes to yield isoxazolinyl-containing β-chiral sulfones bearing quaternary carbon stereocenters with moderate to excellent yields and up to 96:4 er. The advantage and irreplaceability of this sulfur dioxide insertion catalytic system have been demonstrated by achieving transformations clearly unavailable with the previously reported sulfonyl chloride system. Additionally,the recoverability of the new-developed bisoxazoline ligand L9 and its reusability without any erosion of the catalytic activity and enantioselectivity further demonstrate the usefulness of the protocol.

关键词： β-chiral sulfones sulfur dioxide insertion oxysulfonylation copper catalysis enantioselectivity

An approach of the internal friction-dependent temperature changes for conventional and pure biogenic lubricating greases

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Friction 2024年第4期12卷 780-795页

作者： Leif AHME Erik KUHN MiguelÁngel DELGADO department of Mechanical engineering and Production Management Hamburg University of Applied SciencesHamburg 20099Germany department of chemical {2. Research in Product Technology and Chemical Processes(Pro2TecS)University of HuelvaHuelva 21071Spain

This work investigated the temperature changes inside the bulk of lubricating greases under controlled high-shear stress conditions(2.0-500 s-1).For this purpose,a newly developed temperature-measuring cell called Calidus was successfully *** temperature changes(ΔT)have been related to the greases'components(thickener,base oil-type,and composition)and the structural degradation of the lubricating ***,a theoretical approach was proposed for calculating the internal temperature change of lubricating greases during shear *** greases showed an internal temperature profile characterised by a sudden rise inΔT within the first 4 h from starting the test and subsequentΔT decay until it reaches the steady state ***,it was found that greases C1 and C5,formulated with lithium and calcium soap,respectively,with different soap content(16.1 wt%and 9.7 wt%,respectively),but the same base castor oil,showed the highest value of the maximumΔT,c.a.3.2.K,and the most drastic drop ofΔ*** greases showed both the highest specific densities and heat *** addition,they showed the lowest ratio of expended energies(Rtee),which means more structural degradation in the stressed *** the contrary,the grease C3,with 13 wt%of Li-soap but the lowest base oil's viscosity,showed the lowest maximumΔT and the temperature profile was characterised by a moderate variation ofΔT along the *** biogenic grease B3 developed a low-temperature change in the group of pure bio-genic greases close to grease C3.

关键词： shear-induced structural degradation rheology temperature measurements lubricating greases density lubricating greases specific heat capacities