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A Highly Efficient Ni/Al_(2)O_(3)-LaO_(x) Catalyst for the Reductive Amination of Furfural to Furfurylamine:the Promoting Effect of La

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Chemical Research in Chinese Universities 2024年第1期40卷 36-46页

作者： YANG Yinze ZHANG Liyan ZHOU Leilei CHENG Haiyang ZHAO Fengyu State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied chemistry and Engineering University of Science Technology of ChinaHefei 230026P.R.China Jilin Province Key Laboratory of Green chemistry and Process Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China

The reductive amination of furfural to furfurylamine is an important and still challenging topic in the field of biomass conversion. In this work, we prepared a series of Ni/Al_(2)O_(3)-LaO_(x) catalysts by co-precipitation method, the role of La played in promoting the catalytic performances of reductive amination furfural was discussed based on the changes in the electronic state of Ni species, acidity, and Ni particle size. The catalytic activity and the selectivity of furfurylamine are highly dependent on the surface properties and the structure of the catalyst. The addition of La promoted the amount of strong acidic sites and the H2dissociation and spillover on the surface, thus inducing the improvement of the catalytic activity and furfurylamine selectivity. The Ni/Al_(2)O_(3)-0.5LaO_(x)catalyst with suitable acid sites gave a high yield of furfurylamine (94.9%) under mild reaction conditions. Moreover, the catalyst could be recycled five times without significant loss in activity. The Ni/Al_(2)O_(3)-LaO_(x) catalyst is of great promise in the production of amines via reductive amination reaction.

关键词： Reductive amination Furfural Nickel catalyst Furfurylamine Lanthanum

Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of Environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao institute of Catalysis for Energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high photosensitivity.This study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) clusters.To further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and NO.Meanwhile,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate complexes.The H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/mol.The calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational results.Interestingly,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) clusters.Comparison indicted that the chemisorptions of aldehyde oxygen have largest energies.The results suggested adsorption conformations have a respectable impact on the catalysis barrier.This study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

Enhancing zinc-air battery performance by constructing threedimensional N-doped carbon coating multiple valence Co and MnO heterostructures

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Nano Research 2024年第6期17卷 5104-5113页

作者： Qi Liu Panzhe Qiao Miaomiao Tong Ying Xie Xinxin Zhang Kuo Lin Zhijian Liang Lei Wang Honggang Fu Key Laboratory of Superlight Materials and Surface Technology of the Ministry of Education of the People’s Republic of China Harbin Engineering UniversityHarbin 150080China Key Laboratory of Functional inorganic Material chemistry Ministry of Education of the People’s Republic of China Heilongjiang UniversityHarbin 150080China Shanghai institute of Applied Physics Chinese Academy of SciencesShanghai 201204China

Developing highly-efficient bifunctional oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)electrocatalysts is crucial for the widespread application of rechargeable Zn-air batteries(ZABs).Herein,an efficiency electrodeposition and pyrolytic strategy to synthesize the three-dimensional(3D)N-doped carbon coating multiple valence Co and MnO heterostructures supported on carbon cloth substrate(Co-MnO@NC/CC).It contains Co-Co,Co-N,and Co-O bonds,which synergistically enhance the oxygen reaction activity with MnO.It exhibits a working potential of 1.473 V at 10 mA·cm^(−2)for OER and onset potential of 0.97 V for ORR.Theory calculations demonstrate that the synergy between cobalt and manganese species could optimize the d-band center and reduce the energy barrier of Co-MnO@NC/CC for both OER and ORR processes.Besides,the MnO acts as the main OER active site could significantly optimize the energy barrier of O*→OOH*,thus further promoting the OER activity.It can be directly used as the air-cathode for both liquid-state and solid-state ZABs,which could afford a small voltage gap of 0.75 V at 10 mA·cm^(−2),a high power density of 172.5 mW·cm^(−2)and a long-term durability for 400 h,surpassing those of the Pt/C+RuO_(2)-based ZAB.Importantly,the assembled batteries show potential applications in portable devices.

关键词： heterostructure synergy valence cobalt manganese oxide Zn-air battery

Fabrication of Molecularly Imprinted Electrospun Nanofibers with Mono-amidoxime Functional Ligand for Efficient Decontamination of Toxic Organophosphates

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Chinese Journal of Polymer Science 2024年第4期42卷 446-456页

作者： Lan Wang Peng Jiang Ya-Lin Niu Jun-Peng Cao Tian-Ying Guo Key Laboratory of Functional Polymer Materials Ministry of EducationInstitute of Polymer ChemistryCollege of Chemistry and Frontier Science Center for the Creation of New Organic SubstancesNankai UniversityTianjin300071China

There is an urgent imperative to discover practical and efficacious artificial catalysts for the expeditious decontamination of toxic organophosphates. Herein, we propose a novel molecularly imprinted approach utilizing electrospun fiber scaffolds. Specifically, an amidoxime-based functional polymer (PMAOX) has been synthesized, which contains amidoxime groups that can act as nucleophiles and ligands for the formation of catalytic active sites. This polymer was blended with polyacrylonitrile (PAN), a well-processable material, to prepare a nanofiber mat using electrospinning techniques. Then, the amidoxime side groups on fiber surface were further cross-linked after the molecular coordination of templates to complete the molecularly imprinting process. This approach can not only enhance the content of functional molecularly imprinted polymers without affecting structural stability, but also combines surface MI technology to fully expose and leverage the advantages of active sites. The as prepared molecularly imprinted electrospun nanofibers MIF-Zn-PMAOX/PAN-6/4 catalyzes the degradation of paraoxon with a half-life of 32 min, and MIF-Ag-PMAOX/PAN catalyzes the degradation of parathion with a half-life of 18 min. The maximum catalytic rate evidence rate enhancements nearly 3700-fold of the self-hydrolysis. Thus, the mono-amidoxime based molecularly imprinted fibers demonstrate the versatility and superiority as self-detoxifying for organophosphates.

关键词： Organophosphateshydrolysis Electrospinning Molecular imprinting

Bias distribution and regulation in photoelectrochemical overall water-splitting cells

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National Science Review 2024年第4期11卷 141-150页

作者： Kun Dang Siqin Liu Lei Wu Daojian Tang Jing Xue Jiaming Wang Hongwei Ji Chuncheng Chen Yuchao Zhang Jincai Zhao Key Laboratory of Photochemistry CAS ResearchEducation Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences

The water oxidation half-reaction at anodes is always considered the rate-limiting step of overall water splitting（OWS）,but the actual bias distribution between photoanodes and cathodes of photoelectro chemical（PEC） OWS cells has not been investigated systematically.In this work,we find that,for PEC cells consisting of photoanodes（nickel-modified n-Si [Ni/n-Si] and α-Fe2O3） with low photovoltage(Vph 1V,the bias required for cathode activation can be significantly reduced,exhibiting a kinetics-controlled characteristic.Further investigations show that the bias distribution can be regulated by tuning the electrolyte pH and using alternative half-reaction couplings.Accordingly,a volcano plot is presented for the rational design of the overall reactions and unbiased PEC cells.Motivated by this,an unbiased PEC cell consisting of a simple Ni/n-Si photoanode and Pt cathode is assembled,delivering a photo current density of 5.3±0.2 mA cm-2.

关键词： photoelectrochemistry overall reaction cell bias distribution photoanode water splitting

Stabilizing high-efficiency iridium single atoms via lattice confinement for acidic oxygen evolution

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Nano Research 2024年第4期17卷 2492-2498页

作者： Yibo Wang Jiadong Jiang Zhaoping Shi Hongxiang Wu Jiahao Yang Pengbo Wang Shuai Hou Meiling Xiao Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026.China State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Key Laboratory of Physics and Technology for Advanced Batteries Ministry of EducationCollege of PhysicsJilin UniversityChangchun 130012China

Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.

关键词： lattice confinement iridium single atoms ultralow iridium loading acidic oxygen evolution proton exchange membrane water electrolysis

Near-infrared double-cable conjugated polymers based on alkyl linkers with tunable length for single-component organic solar cells

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Chinese Chemical Letters 2024年第4期35卷 452-456页

作者： Yikun Wang Qiaomei Chen Shijie Liang Dongdong Xia Chaowei Zhao Christopher R.McNeill Weiwei Li Beijing Advanced Innovation Center for Soft Matter Science and Engineering&State Key Laboratory of Organic-inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China institute of Applied chemistry Jiangxi Academy of SciencesNanchang 330096China Department of Materials Science and Engineering Monash UniversityWellington RoadClaytonVictoria 3800Australia

The photovoltaic properties of double-cable conjugated polymers are significantly influenced by the length of the alkyl linkers that connect donor backbones and acceptor side units. In this study, a series of 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile(IC)-based double-cable polymers with alkyl linkers ranging from C_8H_(16)to C_(16)H_(32)(Px, x = 8, 10, 12, 14, 16) were synthesized for single-component organic solar cells(SCOSCs). Among these, the linker length x = 12(P12) is found to optimize the power conversion efficiencies(PCEs) in SCOSCs. Specifically, PCEs increase from P8 to P12 and then decline from P12to P16. Detailed investigations of optical absorption, charge transport, and morphology provide insights into the underlying factors contributing to these PCE variations. The findings indicate that the exceptional photovoltaic properties observed in P12 can be attributed to three key factors: A delicate balance between enhanced charge separation facilitated by the increased spacer length and reduced crystallinity resulting from longer spacers, higher charge mobilities, and well-balanced hole/electron transport characteristics. This study highlights the critical role of linker length in determining the photovoltaic properties of double-cable conjugated polymer-based SCOSCs and offers valuable guidance for the design of novel double-cable conjugated polymers.

关键词： Single-component organic solar cells Double-cable conjugated polymers Photovoltaic properties Alkyl linkers

Understanding of the structural evolution of catalysts and identification of active species during CO_(2) conversion

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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao Yifu Yu Department of chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

Printable oil-NiO_(X)hole transport layer enables efficient n-i-p perovskite solar cells with a high thermal stability

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Science China chemistry 2024年第7期67卷 2335-2340页

作者： Yazhou Xu Zhaoyang Chu Hongyu Wang Zhi Xing Baojin Fan Xiaotian Hu Yiwang Chen College of chemistry and Chemical Engineering/institute of Polymers and Energy chemistry(IPEC)/Film Energy chemistry for Jiangxi Provincial Key Laboratory(FEC) Nanchang UniversityNanchang 330031China Key Lab of Fluorine and Silicon for Energy Materials and chemistry of Ministry of Education Jiangxi Normal University Nanchang 330022China Peking University Yangtze Delta institute of Optoelectronics Nantong 226010China

Currently,highly efficient n-i-p perovskite solar cells rely on an organic interface layer for high efficiency,especially 2,2',7,7'-tetrakis[N,N-bis(4-methoxyphenyl)ami-no]-9,9′-spirobifluorene(spiro-OMeTAD),but the instability of organic materials in the photothermal field compromises device stability.In this study,we employ the oleic acid(YS)/oleamine(YA)end-sealing method to achieve uniform dispersion of NiO_(X)nanoparticles,effectively mitigating coagulation resulting from high local concentration and secondary motion adsorption.Furthermore,the conductivity of the hole transport layer and its energy level alignment with perovskite is enhanced by the additional 2,3,5,6-tetrafluoro-7,7',8,8'-tetracyanodimethyl-p-benzoquinone(F4TCNQ),leading to a remarkable improvement of open-circuit voltage and fill factor,thus the high efficiency of 25.17%and 24.36%on 0.1 and 1.01cm2,respectively.Moreover,by realizing an all-inorganic interface layer,an initial efficiency exceeding 90%is maintained even after 2,800 h of heating at 85℃.

关键词： oil-NiO_(X) perovskite solar cells printing technology high efficiency thermal stability