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Boosting the catalytic performance of Cu-SAPO-34in NO_(x) removal via hydrothermal treatment

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Journal of Environmental Sciences 2024年第1期135卷 640-655页

作者： Xiaoyan Tian Huimin Wang Siyuan Xu Lianyun Gao Jinyan Cao Jianjun Chen Qiulin Zhang Ping Ning Jiming Hao Faculty of Environmental Science and Engineering Kunming University of Science and TechnologyKunming 650500China National-Regional Engineering Center for Recovery of Waste Gases from Metallurgical and Chemical industries Kunming University of Science and TechnologyKunming 650500China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China

Phosphate ions promoted Cu-SAPO-34(P-Cu-SAPO-34)were prepared using bulk CuO particles as Cu^(2+)precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO_(x) with NH_3(NH_3-SCR).The effects of high temperature(H-T)hydrothermal aging on the NO_(x) removal(de-NO_(x))performance of Cu-SAPO-34 with and without phosphate ions were systematically investigated at atomic level.The results displayed that both Cu-SAPO-34 and P-Cu-SAPO-34 presented relatively poor NO_(x) removal activity with a low conversion(<30%)at 250-500℃.However,after H-T hydrothermal treatment(800℃ for 10 hr at 10%H_2O),these two samples showed significantly satisfied NO_(x) elimination performance with a quite high conversion(70%-90%)at 250-500℃.Additionally,phosphate ions decoration can further enhance the catalytic performance of Cu-SAPO-34 after hydrothermal treatment(Cu-SAPO-34H).The textural properties,morphologies,structural feature,acidity,redox characteristic,and surface-active species of the fresh and hydrothermally aged samples were analyzed using various characterization methods.The systematical characterization results revealed that increases of 28%of the isolated Cu^(2+)active species(Cu^(2+)-2Z,Cu(OH)^(+)-Z)mainly from bulk CuO and 50%of the Bronsted acid sites,the high dispersion of isolated Cu^(2+)active component as well as the Bronsted acid sites were mainly responsible for the accepted catalytic activity of these two hydrothermally aged samples,especially for P-Cu-SAPO-34H.

关键词： NH_(3)-SCR Cu-SAPO-34 Hydrothermal induced Phosphate ions

Rhodium-catalyzed addition reactions of benzylic C–H bonds to cyclic N-sulfonyl ketimines viaπ-coordination

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Chinese Chemical Letters 2024年第3期35卷 287-291页

作者： Yuntong Li Hang Shi Department of Chemistry Zhejiang UniversityHangzhou 310027China Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province Department of ChemistrySchool of Science and Research Center for Industries of the FutureWestlake UniversityHangzhou 310030China Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024China

Mannich-type reactions are a widely used method for the synthesis of amines due to the readily availability of nucleophiles and electrophiles.However,the inclusion of alkylarenes instead of active carbon pronucleophiles such as aldehydes and ketones in these addition reactions has been a challenge due to the inherent difficulty of benzylic deprotonation.In this study,we present a novel approach for the construction of N-sulfonyl amines via rhodium-catalyzed addition of unbiased benzylic C–H bonds to cyclic N-sulfonyl ketamines throughπ-coordination.This strategy enables the synthesis of a diverse range of N-sulfonyl amines,and subsequent diversification of the addition products showcases the synthetic potential of this protocol.

关键词： Benzylic deprotonation Cyclic N–sulfonyl ketimines π-Coordination Mannich-type addition Rhodium catalysis

Microwave shock motivating the Sr substitution of 2D porous GdFeO_(3) perovskite for highly active oxygen evolution

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Journal of Energy Chemistry 2024年第1期88卷 232-241,I0006页

作者： Jinglin Xian Huiyu Jiang Zhiao Wu Huimin Yu Kaisi Liu Miao Fan Rong Hu Guangyu Fang Liyun Wei Jingyan Cai Weilin Xu Huanyu Jin Jun Wan State Key Laboratory of New Textile Materials and Advanced Processing Technologies Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing&FinishingWuhan Textile UniversityWuhan 430200HubeiChina Future industries Institute STEMUniversity of South AustraliaAdelaideSA 5095Australia Institute for Sustainability Energy and ResourcesThe University of AdelaideAdelaideSA 5005Australia

The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.

关键词： 2D materials Perovskite Microwave Electrocatalysis Oxygen evolution reaction

优化生活用纸生产:争取实现可再生能源项目的高投资回报

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生活用纸 2024年第5期24卷 52-55页

作者： Eduardo De Almeida AFRY Process industries

鉴于电网电力的二氧化碳排放量在29g/kWh~635g/kWh之间浮动,生活用纸生产商正朝着本地可再生能源发电方向发展,本文提出了一个实现工业脱碳的策略。能源成本的上升、环境压力和法规加紧推动着工业企业走向脱碳。然而,在如何实现脱碳生... 详细信息

鉴于电网电力的二氧化碳排放量在29g/kWh~635g/kWh之间浮动,生活用纸生产商正朝着本地可再生能源发电方向发展,本文提出了一个实现工业脱碳的策略。能源成本的上升、环境压力和法规加紧推动着工业企业走向脱碳。然而,在如何实现脱碳生产方面,有多种可选方案。与许多其他工业领域的工厂一样,生活用纸工厂中化石能源的使用是温室气体排放的重要因素。生活用纸行业涵盖了包括纸机生产操作、干燥过程和运输在内的各种环节,均需要投入大量的能源。不同工厂之间的能源来源(例如化石燃料、可再生能源)和能源利用效率可能存在差异,从而影响碳排放情况。

关键词：可再生能源生活用纸纸机生产二氧化碳排放量能源利用效率化石燃料环境压力投资回报

Revealing interfacial charge redistribution of homologous Ru-RuS_(2) heterostructure toward robust hydrogen oxidation reaction

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Journal of Energy Chemistry 2024年第7期94卷 332-339页

作者： Yi Liu Lianrui Cheng Shuqing Zhou Yuting Yang Chenggong Niu Tayirjan Taylor Isimjan Bao Wang Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Saudi Arabia Basic industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.

关键词： Heterostructure Hollow spherical structure Hydrogen oxidation reaction Charge redistribution Density functional calculation

Valence electronic engineering of superhydrophilic Dy-evoked Ni-MOF outperforming RuO_(2) for highly efficient electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2024年第3期90卷 244-252,I0007页

作者： Zhiyang Huang Miao Liao Shifan Zhang Lixia Wang Mingcheng Gao Zuyang Luo Tayirjan Taylor Isimjan Bao Wang Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGulin 541004GuangxiChina State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Saudi Arabia Basic industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.

关键词： Dy@Ni-MOF Dy incorporation Electronic interaction Superhydrophilicity Oxygen evolution reaction

Microwave-assisted exploration of the electron configuration-dependent electrocatalytic urea oxidation activity of 2D porous NiCo_(2)O_(4) spinel

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Journal of Energy Chemistry 2024年第4期91卷 226-235页

作者： Jun Wan Zhiao Wu Guangyu Fang Jinglin Xian Jiao Dai Jiayue Guo Qingxiang Li Yongfei You Kaisi Liu Huimin Yu Weilin Xu Huiyu Jiang Minggui Xia Huanyu Jin State Key Laboratory of New Textile Materials and Advanced Processing Technologies Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing&FinishingWuhan Textile UniversityWuhan 430200HubeiChina Institute for Sustainability Energy and ResourcesThe University of AdelaideAdelaideSA 5005Australia Future industries Institute University of South AustraliaMawson Lakes CampusAdelaideSA 5095Australia

Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.

关键词： 2D materials Spinel Microwave Electrocatalysis Urea oxidation reaction

Cr-catalyzed allylic C(sp^(3))–H addition to aldehydes enabled by photoinduced ligand-to-metal charge transfer

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Science China Chemistry 2024年第5期67卷 1589-1595页

作者： Xianrong Zeng Feng-Hua Zhang Runchen Lai Xiaoyu Lin Zhaobin Wang Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province Department of ChemistrySchool of Science and Research Center for Industries of the FutureWestlake UniversityHangzhou 310030China Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024China Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province Instrumentation and Service Center for Molecular SciencesWestlake UniversityHangzhou 310024China

Photoinduced ligand-to-metal charge transfer(LMCT) has emerged as an effective strategy for synthesizing organic molecules in a sustainable manner. However, the majority of existing reports on selective C(sp^(3))–H bond functionalization via photoinduced LMCT focus on the use of late transition metals or rare-earth metals for radical additions or cross-couplings. In contrast, the utilization of photoinduced LMCT with 3d early transition metals poses a significant challenge. Herein, we describe an unprecedented approach to allylic C(sp^(3))–H addition to aldehydes, employing chromium(Cr) complexes as catalysts through visible-light-induced LMCT. By investigating the reaction pathway through various mechanistic studies, including radical trapping, kinetic isotope effect(KIE) analysis, and transient absorption spectroscopy, valuable insights have been gained. The proposed mechanism suggests the intermediacy of bromine radicals through homolysis of the Cr–Br bond. Notably, this protocol expands our understanding of the photochemical properties of earth-abundant Cr complexes.

关键词： Cr catalysis photoinduced ligand-to-metal charge transfer hydrogen-atom transfer carbonyl addition

Harnessing the power of complex light propagation in multimode fibers for spatially resolved sensing

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Photonics Research 2024年第3期12卷 411-422页

作者： DARCY L.SMITH LINH V.NGUYEN MOHAMMAD I.REJA ERIK P.SCHARTNER HEIKE EBENDORFF-HEIDEPRIEM DAVID J.OTTAWAY STEPHEN C.WARREN-SMITH Institute for Photonics and Advanced Sensing and School of Physics Chemistry and Earth SciencesThe University of AdelaideAdelaideSA 5005Australia Australian Research Council Centre of Excellence for Gravitational Wave Discovery(OzGrav) AdelaideSAAustralia Future industries Institute University of South AustraliaMawson LakesSA 5095Australia Laser Physics and Photonics Devices Laboratory University of South AustraliaMawson LakesSA 5095Australia

The propagation of coherent light in multimode optical fibers results in a speckled output that is both complex and sensitive to environmental effects.These properties can be a powerful tool for sensing,as small perturbations lead to significant changes in the output of the fiber.However,the mechanism to encode spatially resolved sensing information into the speckle pattern and the ability to extract this information are thus far unclear.In this paper,we demonstrate that spatially dependent mode coupling is crucial to achieving spatially resolved measurements.We leverage machine learning to quantitatively extract the spatially resolved sensing information from three fiber types with dramatically different characteristics and demonstrate that the fiber with the highest degree of spatially dependent mode coupling provides the greatest accuracy.

关键词： fiber spatially resolved