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Multiscale confinement nitridation in molybdenum carbide for efficient hydrogen production

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Journal of Energy chemistry 2024年第7期94卷 61-69页

作者： Liming Dai Chenchen Fang Xiaoyuan Zhang Xuefeng Xu Xuanxuan Chen Xinyue Zong Xueming Hu Wenyao Zhang Liang Xue Pan Xiong Yongsheng Fu Jingwen Sun Junwu Zhu key laboratory for Soft chemistry and functional materials Ministry of EducationNanjing University of Science and TechnologyNanjing 210094JiangsuChina

The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.

关键词： Molybdenum carbide Hydrogen evolution reaction Multiscale confinement synthesis Valence band modulation Nitrogen doping

Phosphine-catalyzed acyl-transfer of heteroaryl ketones for the construction of N-fused heterocycles

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Chinese Chemical Letters 2024年第3期35卷 252-256页

作者： Yu Zhang De-Rui Han Dan Ye Hong Lu Hao Wei key laboratory of Synthetic and Natural functional Molecule of the ministry of education College of Chemistry&Materials ScienceNorthwest UniversityXi'an 710069China

An inexpensive phosphine catalyst was used effectively for a transition-metal-free acyl-transfer of N-containing heteroaryl ketones for the rapid synthesis of N-fused heterocycles.The key pre-aromatic spirocyclic intermediate initialized by the single electron transfer(SET)process of Togni's reagentⅡpromoted by the tertiary phosphine resulted in an intriguing and alternative tactic for the cleavage of C–C bonds.By using inexpensive tertiary phosphine as the catalyst,this skeleton-reorganizing approach of N-containing heteroaryl ketones allows a streamlined assembly of complex N-fused heterocycles with broad functional group tolerance.

关键词： Phosphine catalysis Acyl-transfer N-Fused heterocycles C–C bond activation Aromatization

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 process.However,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete insight.Here,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 strategy.The 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,respectively.Furthermore,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 mechanism.This 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

Energy transfer, anticounterfeiting, white light emission and sensing in fine-regulating series of lanthanide metal-organic frameworks

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Journal of Rare Earths 2024年第3期42卷 446-454,I0001页

作者： Juanjuan Xue Yao Wang Guoping Yang Yaoyu Wang key laboratory of Synthetic and Natural functional Molecule chemistry of the ministry of education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi'an710127China

Three lanthanide ions and a rigid(1,1'-biphenyl)-2,4,6-tricarboxylic acid(H_(3)bptc) ligand led to the isostructural lanthanide metal-organic frameworks(Ln-MOFs) {[Ln(bptc)(H_(2)O)_(3)]·3H_(2)O}_n(Lnbptc, Ln = Eu,Tb, Gd, Eu_(x)Tb_(1—x), Eu_(x)Gd_(1-x), Tb_(x)Gd_(1-x), and Eu_(0.12)Tb_(0.52)Gd_(0.36)). The density functional theory(DFT) and time-dependent DFT calculation were expanded on H_3bptc, which point to the occurrence of “antenna effect”. The minor diameter samples of Eubptc, Tbbptc, and Gdbptc can also be attained via the microwave synthesis and employed for handwriting anticounterfeiting. Interestingly, the typical red emission of Eu^(3+) and green emission of Tb~(3+) could be fine-tuned by Gd^(3+) via chemical mixing to be full-color emissions bimetallic doped Eu_(x)Tb_(1-x)bptc, Eu_(x)Gd_(1-x)bptc, and Tb_(x)Gd_(1-x)bptc. The above synthetic bimetallic MOFs can be fixed in positioning boxes of quick response(QR) codes with diverse emission for anticounterfeiting. The message can be decoded under the irradiation of 365 nm ultraviolet lamp while invisible in the daylight. Notably, the trimetallic doped Eu_(0.12)Tb_(0.52)Gd_(0.36)bptc emits white light with the CIE color coordinate(0.34, 0.34). Furthermore, Tbbptc is demonstrated to be a sensitive probe toward nitrobenzene and acetone with multiple mechanisms.

关键词： Metal-organic frameworks Anticounterfeiting White light-emitting Sensing Rare earths

Supramolecular polymer network constructed by a functionalized polyimidazolium salt derived from metal-carbene template approach

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Science China chemistry 2024年第4期67卷 1224-1228页

作者： Ming-Ming Gan Zi-En Zhang Yi-Fan Zhang Heng Zhang Li-Ying Sun Ying-Feng Han key laboratory of Synthetic and Natural functional Molecule chemistry of the ministry of education Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China

In this study,we present a supramolecular templating approach for constructing polyimidazolium salt containing crown ether and cyclobutane moieties.This strategy involves the formation of metal-carbene templates,photochemical cycloaddition,and subsequent demetallation of metal ions.Driven by the host-guest chemistry between crown ether units and ammonium salts,we successfully fabricated a supramolecular polymer SPN1,which features imidazolium receptors and cyclobutane units.The obtained SPN1 demonstrates outstanding reversible stimulus-response,antibacterial behavior and conductivity.

关键词： metal-carbene template crown ether polyimidazolium salt host-guest chemistry

Visible Light-Induced Photocatalysis:Self-Fenton Degradation of p-CIPhOH Over Graphitic Carbon Nitride by a Polyethylenimine Bifunctional Catalyst

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Transactions of Tianjin University 2024年第2期30卷 130-139页

作者： Yuan Bai Shuangjun Li Bolin Yin Jinpeng Zhao Hexing Li key laboratory of Resource chemistry of ministry of education Shanghai Key Laboratory of Rare Earth Functional MaterialsCollege of Chemistry and Materials ScienceShanghai Normal UniversityShanghai 200234China

Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catalyst (Fe-PEI-CN) by codoping graphitic carbon nitride (CN) with polyethyleneimine ethoxylated (PEI) and Fe species, which demonstrated high activity during p-chlorophenol (p-ClPhOH) degradation via H_(2)O_(2) from the photocatalytic process. The relationship between the catalytic efficiency and the structure was explored using diff erent characterization methods. The Fe modification of CN was achieved through Fe-N coordination, which ensured high dispersion of Fe species and strong stability against leaching during liquid- phase reactions. The Fe modification initiated the Fenton reaction by activating H_(2)O_(2) into ·OH radicals for deep degradation of p-ClPhOH. In addition, it eff ectively promoted light absorption and photoelectron-hole (e-h ^(+) ) separation, corresponding to improved photocatalytic activity. On the other hand, PEI could significantly improve the ability of CN to generate H_(2)O_(2) through visible light photocatalysis. The maximum H_(2)O_(2) yield reached up to 102.6 μmol/L, which was 22 times higher than that of primitive CN. The cooperation of photocatalysis and the self-Fenton reaction has led to high-activity mineralizing organic pollutants with strong durability, indicating good potential for practical application in wastewater treatment.

关键词： Fe-PEI-CN bifunctional catalyst Photo-Fenton p-chlorophenol(p-ClPhOH)degradation Synergetic effect

A robust indium-organic framework with open tubular channels for efficient separation of acetylene

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Nano Research 2024年第4期17卷 3139-3146页

作者： Yong-Zhi Li Gang-Ding Wang Fan Xu Qing Yin Danyang Zhao Jiqiu Qi Yanwei Sui Lei Hou Yao-Yu Wang School of materials and physics China University of Mining and TechnologyXuzhou 221116China key laboratory of Synthetic and Natural functional Molecule of the ministry of education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi’an 710069China

Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring challenge.Herein,we designed and synthesized a robust three-dimensional(3D)indium-organic framework([(Me)_(2)NH_(2)][In(L6)_(0.5)(IPA)_(0.5)]·DMA·2H_(2)O(In-L6-IPA,DMA=dimethylammonium,IPA=isopropyl alcohol))featuring two types of one-dimensional(1D)tubular channels.The activated In-L6-IPA displayed high loading for C_(2)H_(2)(104.4 cm^(3)·g^(-1),the second highest value among all reported indium-based metal-organic frameworks(MOFs))and simultaneously selective adsorption for C_(2)H_(2) over CO_(2),C_(2)H_(6),and ethylene(C_(2)H_(4))at 298 K under 100 kPa.Molecular modelling revealed that the porous wall of In-L6-IPA provides more and stronger multiple interactions for C_(2)H_(2) than CO_(2),C_(2)H_(6),and C_(2)H_(4) containing C–H···π,C–H···O,and O···πinteractions.Breakthrough experiments validated the actual separation ability for various ratios of binary C_(2)H_(2)/C_(2)H_(4) and C_(2)H_(2)/CO_(2) mixtures as well as equimolar ternary C_(2)H_(2)/C_(2)H_(4)/CO_(2) and C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6) mixtures with excellent reusability.

关键词： indium-organic framework crystal structure gas adsorption acetylene(C_(2)H_(2))separation

Engineering of geometrical configurations in dual-atom catalysts for electrocatalytic applications

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Journal of Energy chemistry 2024年第7期94卷 273-287页

作者： Tao Zhang Yifan Liu Liang Xue Jingwen Sun Pan Xiong Junwu Zhu key laboratory for Soft chemistry and functional materials of ministry education School of Chemistry and Chemical EngineeringNanjing University of Science and TechnologyNanjing210094JiangsuChina

Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,but in-depth understanding the relationship between geometrical configurations and metal-metal interaction mechanisms for designing targeted DACs is still required.In this review,the recent progress in engineering of geometrical configurations of DACs is systematically summarized.Based on the polarity of geometrical configuration,DACs can be classified into two different types that are homonuclear and heteronuclear DACs.Furthermore,with regard to the geometrical configurations of the active sites,homonuclear DACs are identified into adjacent and bridged configurations,and heteronuclear DACs can be classified into adjacent,bridged,and separated configurations.Subsequently,metal-metal interactions in DACs with different geometrical configurations are introduced.Additionally,the applications of DACs in different electrocatalytic reactions are discussed,including the oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER),and other catalysis.Finally,the future challenges and perspectives for advancements in DACs are high-lighted.This review aims to provide inspiration for the design of highly effcient DACs towards energy relatedapplications.

关键词： Dual-atom catalysts Geometrical configurations Homonuclear Heteronuclear Electrocatalysis

Open-Shell Oligomers and Polymers: Theory, Characterization Methods, Molecular Design, and Applications

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Chinese Journal of Polymer Science 2024年第4期42卷 417-436页

作者： Xue-Qing Wang Cheng Song Ting Lei key laboratory of Polymer chemistry and physics(ministry of education) School of Materials Science and EngineeringPeking UniversityBeijing100871China

Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFETs), photodetectors, organic thermoelectrics, and spintronics. Although open-shell ground states have been observed in certain small molecules and doped organic semiconductors, the exploration of open-shell ground-state conjugated polymers is still limited, and the strategies for designing these polymers remain obscure. This review aims to briefly introduce the theory and characterization methods of open-shell conjugated polymers, along with an overview of recent progress and applications. The objective is to stimulate further advancements and investigations in this promising area by shedding light on the potential of open-shell conjugated polymers and the challenges that lie ahead.

关键词： Conjugated polymers Open-shell molecules High-spin ground state Donor-acceptor(D-A)polymers Optoelectronic and magnetic properties