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Chinese Chemical Letters 2024年第2期35卷 611-616页

作者： Jiawen Sun Hui Xue Jing Sun Niankun Guo Tianshan Song Yi-Ru Hao Qin Wang college of chemistry and Chemical engineering Inner Mongolia UniversityHohhot 010021China

Modulating surface charge redistribution based on interface and defect engineering has been considered as a resultful means to boost electrocatalytic ***,the mechanism of synergistic regulation of heterojunction and vacancy defects remains ***,a Vs-CoP-CoS_(2)/C n-n heterojunction with sulfur vacancies is successfully constructed,which manifests superior electrocatalytic activity for oxygen evolution,as demonstrated by a low overpotential of 170 mV to reach 10 mA/cm^(2).The experimental results and density functional theory calculations testify that the outstanding OER performance of Vs-CoP-CoS_(2)/C heterojunction is owed to the synergistic effect of sulfur vacancies and built-in electric field at n-n heterogeneous interface,which accelerates the electron transfer,induces the charge redistribution,and regulates the adsorption energy of active intermediates during the *** study affords a promising means to regulate the electrocatalytic performance by the construction of heterogeneous interfaces and defects,and in-depth explores the synergistic mechanisms of n-n heterojunction and vacancies.

关键词： Charge redistribution n-n Heterojunction Built-in electric field Sulfur vacancy Oxygen evolution reaction

Matrix-Mediated Color-Tunable Ultralong Organic Room Temperature Phosphorescence of 7H-Benzo[c]carbazole Derivatives

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CCS chemistry 2024年第3期6卷 798-811页

作者： Chen Qian Xue Zhang Zhimin Ma Xiaohua Fu Zewei Li Huiwen Jin Mingxing Chen Hong Jiang Zhiyong Ma Beijing Advanced Innovation Center for Soft Matter Science and engineering State Key Laboratory of Organic–Inorganic CompositesCollege of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029 Beijing National Laboratory for molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871

Building on the recent systematic research on 1Hbenzo[f]indole(Bd),an important advancement in constructing ultralong organic room temperature(UORTP)materials with a universal strategy via a readily obtained unit(7H-Benzo[c]carbazole,BCz)is proposed in this *** powders of BCz and its derivatives merely exhibit blue fluorescence at ambient ***,when BCz and its derivatives are dispersed into polymer or powder matrixes,strong photo-activated green UORTP can be observed from their doped systems at room ***,the UORTP color can be tuned between green and yellow depending on the *** ultralong phosphorescence originates from the generation of charge-separated states via *** matrixes play a key role in both stabilizing charge-separated states and controlling UORTP *** interestingly,when using polymethyl methacrylate as matrix,the doped films achieve stronger photo-activated ultralong phosphorescence underwater than in air at room *** Bd,BCz achieves better performance not only in ultralong phosphorescence properties but also in practical *** work gains a deeper insight into the mechanism of UORTP and paves a new approach to applying organic phosphorescent materials to underwater coating and imaging.

关键词： 7H-Benzo[c]carbazole ultralong organic room temperature phosphorescence ion radical matrix-mediated color tunning underwater application

Synergy of phosphorus vacancies and build-in electric field into NiCo/NiCoP Mott-Schottky integrated electrode for enhanced water splitting performance

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Chinese Chemical Letters 2024年第2期35卷 604-610页

作者： Xiaochen Zhang Hui Xue Jing Sun Niankun Guo Tianshan Song Jiawen Sun Yi-Ru Hao Qin Wang college of chemistry and Chemical engineering Inner Mongolia UniversityHohhot 010021China

Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorption energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for improving catalytic ***,the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains ***,the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel(NF)has been synthesized through continuous phosphating and reduction *** obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities,and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm^(2) in 1 mol/L KOH,***,as both the cathode and anode of overall water splitting,the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm^(2),which are far exceeding the benchmark commercial *** theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor,tailor the electronic structure of the metal centers and lower the Gibbs free energy of the ***,the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site,avoid catalyst shedding,thus improving the activity and structural stability of NiCo/*** study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.

关键词： Mott-Schottky Build-in electric field Phosphorus vacancies Phosphides Overall water splitting

Ternary-phase layered cathodes toward ultra-stable and highrate sodium ion storage

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Rare Metals 2024年第4期43卷 1589-1598页

作者： Wen-Ji Yin Pei-Dan Su Qi Lu Xiao-Qiong Li Ji-Ming Peng Teng-Fei Zhou Ge-Meng Liang Yu-Liang Cao Hong-Qiang Wang Qing-Yu Li Si-Jiang Hu Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin541004China Institutes of Physical Science and Information Technology Anhui UniversityHefei230601China Department of chemistry and Pharmaceutical Sciences Guilin Normal CollegeGuilin541199China college of chemistry and Chemical engineering Huanggang Normal UniversityHuanggang438000China School of Chemical engineering and Advanced Materials The University of AdelaideAdelaide5005Australia engineering Research Center of Organosilicon Compounds and Materials of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan430072China

With the shortage of lithium resources,sodiumion batteries(SIBs)are considered one of the most promising candidates for lithium-ion batteries.P2-type and O3-type layered oxides are one of the few cathodes that can access high energy ***,they usually exhibit structural change,capacity decay,and slow Na ion ***,we present layered ternary-phase cathodes with P2,P3 and O3 phases by a lattice doping strategy,which is demonstrated by X-ray diffraction(XRD)*** the characteristics of P2,P3 and O3 phases,the layered composites show performance improvement during long-term battery *** particular,Na_(0.7)Li_(0.1)Co_(0.3-)Fe_(0.3)Mn_(0.3)O_(2)(NLCFM)delivers a reversible capacity of120.1 mAh·g^(-1)at 0.1C(1.0C=175 mA·g^(-1))with a superior capacity retention of 72.5%after 1000 cycles *** work offers insights into the development of advanced cathode materials for SIBs.

关键词： Sodium-ion battery Cathode material Layered oxides Lattice doping Mixed phase

Synergetic Bioproduction of Short-Chain Fatty Acids from Waste Activated Sludge Intensified by the Combined Use of Potassium Ferrate and Biosurfactants

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Journal of Ocean University of China 2024年第3期23卷 695-709页

作者： CHEN Yanyan YAO Shuo ZHANG Dahai LI Xianguo FENG Lijuan college of chemistry and Chemical engineering Ocean University of ChinaQingdao 266100China

The synergetic effect and underlying mechanism of potassium ferrate(PF)with tea saponin(TS,a biosurfactant)in producing short chain fatty acids(SCFAs)from anaerobic fermentation of waste activated sludge(WAS)were explored in this *** results showed that 0.2 g PF(g TSS)^(-1)(total suspended solid)combined with 0.02 g TS(g TSS)^(-1) could further improve SCFAs’production,and the maximum SCFAs content reached 2008.7 mg COD L^(-1),which is 1.2 and 4.5 times higher than those with PF and TS individually added,respectively,and 5.3 times higher than that of blank WAS on Day *** the model substrates experiments,the degradation rates of bovine serum albumin and dextran with combination of PF and TS were 41.3%±0.1% and 48.5%±0.06%,respectively,on Day 3,which are lower than those in blank WAS(with degradation rates of 72.3%±0.5%and 90.3%±0.3%).It was revealed that the oxidative effect of PF and the solubilization of TS caused more organic matters to be dissolved out from WAS,providing a large number of biodegradable substances for subsequent SCFAs *** WAS pretreated with the combination of PF and TS,the relative abundances of Firmicutes increased from 6.4%(blank)to 38.6%,and that of Proteobacteria decreased from 41.8%(blank)to 21.8%.The combination of PF and TS promoted the hydrolysis process of WAS by enriching Firmicutes,and then increased acetic acid production by inhibiting Proteobacteria that consumed ***,at the genus level,acidogenesis bacteria(e.g.,Proteiniclasticum and Petrimonas)were enriched whereas SCFAs consuming bacteria(e.g.,Dokdonella)were inhibited.

关键词： waste activated sludge anaerobic fermentation potassium ferrate biosurfactant pretreatment

Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

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Nano Research 2024年第4期17卷 3413-3422页

作者： Huimei Chen Yan Yang Chi Jiao Zhiwen Zhuo Junjie Mao Yan Liu Key Laboratory of Functional molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China

The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch ***,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete ***,a series of graphene-based N-bridged dual-atom catalysts(M1-N-M2/NC)are systematically investigated via first-principle calculation and a high-throughput screening *** result unveils that N_(2) adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts(SACs).Moreover,V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts,with extremely low limiting potentials of-0.20 and-0.18 V,***,the adsorption site competition between*N_(2) and*H,as well as the competitive twin reactions of hydrogen evolution reaction(HER)on intermediates(N_(n)H_(m))during the e-NRR process,is systematically evaluated to form a remodeling insight for the reactions in mechanism,and the e-NRR of new proposed dual-atom catalysts(DACs)is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR *** work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.

关键词： nitrogen reduction dual-atom catalysts high-throughput screening hydrogen evolution reaction density functional theory calculations

Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

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Nano Research 2024年第6期17卷 5298-5304页

作者： Yuwei He Yueguang Chen Renjie Wu Zhihe Xiao Mengxian Li Chunfeng Shi Leyu Wang State Key Laboratory of Chemical Resource engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of Petroleum molecular and Process engineering SINOPEC Research Institute of Petroleum Processing Co.Beijing 100083China

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains ***,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the *** NWs possess uniform sizes and well-controlled atomic *** to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based ***,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/*** ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.

关键词： ligand effect oxygen reduction reaction group VI B transition metal ultrathin nanowires multiple oxygen species

Copper-Catalyzed Hydrogen Production through the Dehydrogenative Coupling of Methanol and Diamine Published as part of Precision chemistry virtual special issue “Precision chemistry for the Hydrogen Cycle”

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Precision chemistry 2024年第4期2卷 138-142页

作者： Danyang Cheng Shixiang Yu Meng Wang Ding Ma Beijing National Laboratory for molecular Sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

A hydrogen storage system was developed via heterogeneous catalysis,employing the dehydrogenative coupling of methanol and N,N′-dimethylethylenediamine to efficiently produce high-purity H_(2).In this process,the Cu/ZnO/Al_(2)O_(3) catalyst displayed superior activity in hydrogen production,with Cu+identified as the major active site through comprehensive characterization.

关键词： methanol reforming hydrogen release aminocarbonylation dehydrogenative coupling Cu/ZnO/Al_(2)O_(3)catalyst

Synthesis of Long-Chain Oligomeric Donor and Acceptors via Direct Arylation for Organic Solar Cells

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Chinese Journal of chemistry 2024年第5期42卷 523-532页

作者： Yu Wu Xin-Yu He Xu-Min Huang Ling-Jun Yang Peng Liu Na Chen Chang-Zhi Li Shi-Yong Liu Jiangxi Provincial Key Laboratory of Functional molecular Materials chemistry College of MaterialsMetallurgical and ChemistryJiangxi University of Science and TechnologyGanzhouJiangxi341000 China Department of Polymer Science and engineering Zhejiang UniversityHangzhouZhejiang310027 China

The rapid synthesis of structurally complicated electron donors&acceptors still remains a major challenge in organic solar cells(OSC).In this work,we developed a highly efficient strategy to access long-chain oligomeric donor and acceptors for OSC applications.A series of cyclopentadithiophene(CPDT)and benzothiadiazole(BT)-basedπ-conjugated oligomers,i.e.,three oligomeric acceptors(BTDT)n-IC(n=1—3)and one long-chain oligomeric donor(BTDT)4-RD,are facilely synthesized by an atom-and step-economical,and labor-saving direct C—H arylation(DACH)reaction(i.e.,C—H/C—Br cross coupling).Note that(BTDT)4-RD involving five CPDT,four BT and two rhodamine(RD)building blocks is the longest oligomeric donor in the fullerene-free OSC devices ever *** dependence of the structure-property-performance correlation of(BTDT)n-IC(n=1—3)and(BTDT)4-RD on theπ-conjugation lengths is thoroughly investigated by opto-electrochemical measurements,bulk heterojunction(BHJ)OSC devices and ***(BTDT)1-IC:PBDB-T and(BTDT)4-RD:Y6 BHJs achieve power conversion efficiencies of 9.14%and 4.51%,*** findings demonstrate that DACH reaction is a powerful tool to tune the opto-electronic properties and device performances by regulating the lengths ofπ-conjugated oligomers with varied numbers of repeating units.

关键词： Long-chainπ-conjugated oligomer Organic solar cells Direct arylation Atom-economical synthesis Cyclopentadithiophene Benzothiadiazole C—H activation Conjugation Oligomers