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Nano Research 2024年第9期17卷 8552-8559页

作者： Donghao Zhang Lianxi Si Qianqian Ren Xintong Yan Shi Hu Department of Chemistry School of ScienceTianjin Key Laboratory of Molecular Optoelectronic ScienceTianjin UniversityTianjin 300072China

Pd-based catalysts exhibit higher catalytic activity and durability in many electrochemical ***,the electrochemical performance can be further enhanced by fine-tune of the alloy *** binary alloys have been fully studied,the multicomponent alloys are far beyond understanding,which leaves cocktail effect a compromised explanation for the high-entropy *** Pd nanosheet-seeded growth was used to synthesize a Pd-Zn-Cd ternary alloy by accurately controlling the Pd-Zn-Cd molar ratio through adjusting the amount of introduced Cd *** analysis of the crystal phase structure of PdCdZnx and PdZn_(x)Cd_(1-x),the competitive relationship of Zn and Cd in the alloying process with Pd was unveiled:Pd1Cd1 intermetallics(IMC)is thermodynamically favored over Pd_(1)Zn_(1)IMC in the ternary ***,the increased structure stability of PdCd over PdZn does not bring about increased durability in the catalytic ethanol oxidation *** morphology selection of Pd seeds is also crucial for the study,as Pd cubes,Pd tetrahedrons,and Pd octahedrons do not form PdZn in the same *** successful alloying through the seeded growth depends on the maximum diffusion depth of foreign atoms into the seed.

关键词： PdZn alloy seed growth method ethanol oxidation reaction composition control ternary alloying

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

Heterocatalytic ethylene methoxycarbonylation via a pseudo-hydride pathway over Pt_(1)/MoS_(2)

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science China Chemistry 2024年第8期67卷 2427-2428页

作者： Bo-Hang Zhao Bin Zhang Institute of molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Ethylene (C2H4) methoxycarbonylation (EMC) with CO and methanol (CH3OH) to methyl propanoate (MP) is industrially important due to its 100% atom efficiency [1].However, the heavy reliance on homogeneous Pd-based catalysts and strong acid media over commercial EMC processes still causes economic and environmental concerns [2]. At present, supported single-atom catalysts (SACs) can serve as bridges for accessing homogeneous catalysts in traditional heterogeneous catalytic processes.

关键词： processes. catalytic hydride

Catalysis by subsurface metal atoms in Al(001) through electron transfer

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National science Review 2024年第4期11卷 12-13页

作者： Bo Sun Ding Ma Beijing National Laboratory for molecular science New Cornerstone Science Laboratory College of Chemistry and Molecular Engineering Peking University

Heterogeneous catalysis plays a crucial role in the chemical industry, which has evolved from the investigation of chemisorption to an electronic structure[1]. Diverse strategies, such as alloying,doping, and confining, have been applied to enhance the catalytic properties of active sites through electronic modulation. The electron transfer between active sites and substrates profoundly influences catalytic activity [2].

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Enhanced Ethylene Production from Electrocatalytic Acetylene Semi-hydrogenation Over Porous Carbon-Supported Cu Nanoparticles

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Transactions of Tianjin University 2024年第4期30卷 297-304页

作者： Li Li Fanpeng Chen Bo-Hang Zhao Yifu Yu Institute of molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Electrocatalytic semi-hydrogenation of acetylene(C_(2)H_(2))over copper nanoparticles(Cu NPs)offers a promising non-petroleum alternative for the green production of ethylene(C2H4).However,server hydrogen evolution reaction(HER)competition in this process prominently decreases C2H4 selectivity,thereby hindering its practical ***,a Cu-based composite catalyst,wherein porous carbon with nanoscale pores was used as a support,is constructed to gather the C_(2)H_(2) feedstocks for suppressing the undesirable *** a result,the as-prepared catalyst exhibited C_(2)H_(2) conversion of 27.1%and C_(2)H_(4) selectivity of 88.4%at a C2H4 partial current density of 0.25 A/cm^(2) under optimal−1.0 V versus reversible hydrogen electrode(RHE)under the simulated coal-derived C_(2)H_(2) atmosphere,significantly outperforming the single Cu NPs *** addition,a series of in situ and ex situ experimental results show that not only the porous nature of the carbon support but also the stabilized Cu^(0)–Cu^(+) dual active sites through the strong metal–support interactions enhance the adsorption capacity of C_(2)H_(2),leading to high C_(2)H_(2) partial pressure,restraining the HER and thus improving the C2H4 selectivity.

关键词： Electrocatalysis Cu-based catalyst Hydrogenation Ethylene Selectivity

Superatom-assembled boranes,carboranes,and low-dimensional boron nanomaterials based on aromatic icosahedral B_(12)and C_(2)B_(10)

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Nano Research 2024年第7期17卷 6734-6740页

作者： Qiao-Qiao Yan Yan-Fang Wei Qiang Chen Yue-Wen Mu Si-Dian Li Institute of molecular science Shanxi UniversityTaiyuan 030006China

Using the experimentally known aromatic icosahedral superatoms I_(h)B_(12)H_(12)2−and D_(5d)1,12-C_(2)B_(10)H_(12)as building blocks and based on extensive density functional theory calculations,we predict herein a series of core–shell superpolyhedral boranes and carboranes in a bottom-up approach,including the high-symmetry Th B_(12)@B_(152)H_(72)2−(2),C2h C_(2)B_(10)@B_(152)H_(72)(3),D_(3d)B_(12)@B_(144)H_(66)(4),I_(h)B_(12)@C_(24)B_(12)0H_(72)2−(6),and D_(5d)C_(2)B_(10)@C_(24)B_(12)0H_(72)(7).More interestingly,the superatom-assembled linear D2h B_(36)H_(32)^(2−)(8),close-packed planar D_(3d)B_(84)H_(60)^(2−)(10),and nearly close-packed core−shell D_(3d)B_(12)@B144H_(6)6(4)can be extended periodically to form the one-dimensional(1D)α-rhombohedral borane nanowire B_(12)H_(10)(Pmmm)(9),two-dimensional(2D)α-rhombohedral monolayer borophane B_(12)H_(6)(P m1)(11),and the experimentally known three-dimensional(3D)α-rhombohedral boron(R m)(12)which can be viewed as an assembly of the monolayer B_(12)H_(6)(11)staggered in vertical direction,setting up a bottom-up strategy to form low-dimensional boron-based nanomaterials from their borane“seeds”via partial or complete *** bonding analyses indicate that the high stability of these nanostructures originates from the spherical aromaticity of their icosahedral B_(12)or C_(2)B_(10)structural units which possess the universal skeleton electronic configuration of 1S21P61D101F8 following the Wade’s n+1 *** infrared(IR)and Raman spectra of the most-concerned neutral B_(12)@B144H_(6)6(4)and C_(2)B_(10)@C_(24)B_(12)0H_(72)(7)are computationally simulated to facilitate their experimental characterizations.

关键词： superatom-assembling bottom-up approach density functional theory superpolyhedral boranes superpolyhedral carboranes borophanes

Oxidation Evolution and Activity Origin of N-Doped Carbon in the Oxygen Reduction Reaction

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Transactions of Tianjin University 2024年第4期30卷 369-379页

作者： Jiaqi Wu Chuanqi Cheng Shanshan Lu Bin Zhang Yanmei Shi Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China school of Materials science and Engineering Institute of New Energy MaterialsTianjin UniversityTianjin 300072China Tianjin Key Laboratory of molecular Optoelectronic science Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China

N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively ***,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon ***,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not *** this study,we discover a two-step oxida-tion process of N-doped carbon during the *** fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional *** oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)***,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant *** also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.

关键词： Oxygen reduction reaction N-doped carbon Reaction path Structural evolution Oxidation in reduction

Bridging molecular photosensitizer and catalyst on carbon nanotubes toward enhanced selectivity and durability for CO_(2)photoreduction

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Journal of Environmental sciences 2024年第6期140卷 157-164页

作者： Xiaofeng Cui Xueting Wang Lijun Zhao Jixin Wang Tingting Kong Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China school of Chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246011China school of Chemistry and Materials science University of Science and Technology of ChinaHefei 230026China

Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and ***,their low durability and recyclability limit practical *** this work,we immobilized the catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous *** characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular catalysts are anchored,which is three times higher than that of homogeneous molecular ***,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly *** work provides an effective pathway for constructing heterogeneous photocatalysts based on rational assembly of efficient molecular photosensitizers and catalysts.

关键词： durability selectivity catalyst

Simultaneous Bulk-and Surface-initiated Living Polymerization Studied with a Heterogeneous Stochastic Reaction Model

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Chinese Journal of Polymer science 2024年第3期42卷 364-372,I0008页

作者： Jia-Shu Ma Zhi-Ning Huang Jia-Hao Li Bang-Ping Jiang Yan-Da Liao Shi-Chen Ji Xing-Can Shen State Key Laboratory for Chemistry and molecular Engineering of Medicinal Resources Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources(Ministry of Education of China)School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004China school of Computer science and Engineering&school of Software Guangxi Normal UniversityGuilin 541004China

To better characterize the properties of surface-initiated polymers, simultaneous bulk-and surface-initiated polymerizations are usually carried out by assuming that the properties of the surface-initiated polymers resemble those of the bulk-initiated polymers. Through a Monte Carlo simulation using a heterogeneous stochastic reaction model, it was discovered that the bulk-initiated polymers exhibit a higher molecular weight and a lower dispersity than the corresponding surface-initiated polymers, which indicates that the equivalent assumption is invalid. Furthermore, the molecular weight distributions of the two types of polymers are also different, suggesting different polymerization mechanisms. The results can be simply explained by the heterogeneous distributions of reactants in the system. This study is helpful to better understand surface-initiated polymerization.

关键词： Surface-initiated polymerization Polymer brush Stochastic reaction model Heterogeneous polymerization Simultaneous polymerization

Polymer: Non-fullerene acceptor heterojunction-based phototransistor for short-wave infrared photodetection

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Nano Research 2024年第4期17卷 3087-3095页

作者： Jing Li Weigang Zhu Yang Han Yanhou Geng Wenping Hu Key Laboratory of Organic Integrated Circuits of Ministry of Education&Key Laboratory of molecular Optoelectronic sciences School of Science&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China Key Laboratory of Organic Integrated Circuits of Ministry of Education&Key Laboratory of molecular Optoelectronic sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

It remains full of challenge for extending short-wave infrared(SWIR)spectral response and weak-light detection in the context of broad spectral responses for *** this work,a novel poly(2,5-bis(4-hexyldodecyl)-2,5-dihydro-3,6-di-2-thienyl-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thiophene)(PDPPT3-HDO):COTIC-4F organic bulk-heterojunction is prepared as active layer for bulk heterojunction ***3-HDO serves as a hole transport material,while COTIC-4F enhances the absorption of SWIR light to 1020 *** a result,smooth and connected PDPPT3-HDO film is fabricated by blade coating method and exhibits high hole mobility up to 2.34 cm^(2)·V^(-1)·s^(-1) with a current on/off ratio of 4.72×10^(5) in organic thin film ***3-HDO:COTIC-4F heterojunction phototransistors exhibit high responsivity of 2680 A·W^(-1) to 900 nm and 815 A·W^(-1) to 1020 nm,with fast response time(rise time~20 ms and fall time~100 ms).The photosensitivity of the heterojunction phototransistor improves as the mass ratio of non-fullerene acceptors increases,resulting in an approximately two orders of magnitude enhancement compared to the bare polymer ***,the phototransistor exhibits decent responsivity even under ultra-weak light power of 43μW·cm^(-2) to 1020 *** work represents a highly effective and general strategy for fabricating efficient and sensitive SWIR light photodetectors.

关键词： photodetection phototransistor organic semiconductor heterojunction non-fullerene acceptor