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Catalytic oxidation of toluene by manganese oxides:Effect of K^(+)doping on oxygen vacancy

Journal of Environmental Sciences 2024年第8期142卷 43-56页

作者： Zhenzhen huang haiyang Li Xuejun Zhang Yanli mao Yinghan Wu Wei Liu hongrun Gao Mengru Zhang Zhongxian Song Faculty of Environmental and Municipal Engineering Henan Key Laboratory of Water Pollution Control and Rehabilitation TechnologyHenan University of Urban ConstructionPingdingshan 467036China College of Environmental and Safety Engineering Shenyang University of Chemical TechnologyShenyang 110142China

Alkali metal potassium was beneficial to the electronic regulation and structural stability of transition metal ***,K ions were introduced into manganese oxides by different methods to improve the degradation efficiency of *** results of activity experiments indicated that KMnO_(4)-hT(hT:hydrothermal method)exhibited outstanding low-temperature catalytic activity,and 90%conversion of toluene can be achieved at 243℃,which was 41℃and 43℃lower than that of KNO_(3)-hT and Mn-hT,*** largest specific surface area was observed on KMnO_(4)-hT,facilitating the adsorption of *** formation of cryptomelane structure over KMnO_(4)-hT could contribute to higher content of Mn^(3+)and lattice oxygen(Olatt),excellent low-temperature reducibility,and high oxygen mobility,which could increase the catalytic ***,two distinct degradation pathways were ***Ⅰ(KMnO_(4)-hT):toluene→benzyl→benzoic acid→carbonate→CO_(2)and h2O;PathwayⅡ(Mn-hT):toluene→benzyl alcohol→benzoic acid→phenol→maleic anhydride→CO_(2)and *** intermediates were detected on KMnO_(4)-hT,indicating its stronger oxidation capacity of toluene,which was originated from the doping of K^(+)and the interaction between *** intermediates were observed on Mn-hT,which can be attributed to the weaker oxidation ability of pure *** results indicated that the doping of K^(+)can improve the catalytic oxidation capacity of toluene,resulting in promoted degradation of intermediates during the oxidation of toluene.

关键词： Catalytic oxidation Preparation method Cryptomelane Mn^(3+)and lattice oxygen

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Effects of water molecules on luminescence in europium and terbium coordination polymers with p-fluorobenzoic acid as ligand

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Journal of Rare Earths 2024年第7期42卷 1258-1264,I0003页

作者： Xiaoqi Zhao Puyan hao Yami Ling Mengzhen Jia Rui Zhu Jiawen Liu qiang Xu Jianhong Zhou Collaborative Innovation Center of Rare-Earth Optical Functional Materials and Devices Development Baoji Key Laboratory of Micro-Nano Optoelectronics and Terahertz TechnologySchool of Physics and Opto-Electronic TechnologyBaoji University of Arts and SciencesBaoji721016China

Our previous experimental observations show that the crystal structure of lanthanide luminescent complexes synthesized in aqueous solution usually contains a large number of coordination water molecules or free water *** order to probe the influence of water molecules on luminescent processes of lanthanide complexes,the photoluminescence properties of Ln-FBA(Ln=Eu and Tb,FBA=p-fluorobenzoic acid)coordination polymers at different ambient temperatures,in different solvents and aqueous DMSO solutions with different volume concentrations were systematically *** experiment results show that the presence of water molecules can promote the energy transfer from FBA ligand to Ln3+,at the same time,can cause luminescent non-radiation quenching of lanthanide *** addition,the variation of emission intensity ratio of 615 nm/591 nm peaks of Eu^(3+)with increasing the volume concentration of h_(2)O can be potentially used for the quantitatively detection of water traces in organic *** order to suppress the non-radiation quenching caused by the water molecules,Ln-FBA(Ln=Eu and Tb)coordination polymers were embedded into the PVP matrix to prepare Ln-FBA@PVP hybrid *** photoluminescence investigation indicates that PVP can not only block the quenching effect of water molecules on luminescence,but also effectively sensitize Eu^(3+)and Tb^(3+)*** experimental conclusions are useful for probing the influence of water molecules on luminescent processes of lanthanide complexes,quantitatively detecting water traces in organic solvents and enhancing the photoluminescence intensity in lanthanide complexes.

关键词： Lanthanide complexes Photoluminescence Luminescent quenching Rare earths

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Boosting oxygen reduction activity and CO_(2) resistance on bismuth ferrite-based perovskite cathode for low-temperature solid oxide fuel cells below 600℃

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Journal of Energy Chemistry 2024年第3期90卷 600-609,I0013页

作者： Juntao Gao Zhiyun Wei Mengke Yuan Zhe Wang Zhe Lü qiang Li Lingling Xu Bo Wei School of Physics Harbin Institute of TechnologyHarbin 150001HeilongjiangChina Key Laboratory of Functional Inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina School of Physics and Electronic Engineering Harbin Normal UniversityHarbin 150025HeilongjiangChina

Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical ***,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for *** doping can significantly enhance the electrocata lytic activity and chemical stability of *** 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious *** remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi ***,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) *** work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.

关键词： Low-temperature solid oxide fuel cell Perovskite cathode DFT calculations CO_(2) tolerance

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Multiscale analysis of fine slag from pulverized coal gasification in entrained-flow bed

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International Journal of Coal Science & Technology 2024年第1期11卷 119-132页

作者： Lirui mao Mingdong Zheng Baoliang Xia Facun Jiao Tao Liu Yuanchun Zhang Shengtao Gao hanxu Li School of Chemical Engineering Anhui University of Science and TechnologyHuainan232001China School of Earth and Environment Anhui University of Science and TechnologyHuainan232001China Insititute of Energy Hefei Comprehensive National Science CenterHefei230031China

Fine slag(FS)is an unavoidable by-product of coal ***,which is a simple heap of solid waste left in the open air,easily causes environmental pollution and has a low resource utilization rate,thereby restricting the development of energy-saving coal gasification *** multiscale analysis of FS performed in this study indicates typical grain size distribution,composition,crystalline structure,and chemical bonding *** FS primarily contained inorganic and carbon components(dry bases)and exhibited a"three-peak distribution"of the grain size and regular spheroidal as well as irregular *** irregular particles were mainly adsorbed onto the structure and had a dense distribution and multiple pores and *** carbon constituents were primarily amorphous in structure,with a certain degree of order and active sites.C 1s XPS spectrum indicated the presence of C–C and C–h bonds and numerous aromatic *** inorganic components,constituting 90%of the total sample,were primarily silicon,aluminum,iron,and *** inorganic components contained Si–O-Si,Si–O–Al,Si–O,SO_(4)^(2−),and Fe–O *** 2p XPS spectrum could be deconvoluted into Fe 2p_(1/2) and Fe 2p_(3/2) peaks and satellite peaks,while Fe existed mainly in the form of Fe(III).The findings of this study will be beneficial in resource utilization and formation mechanism of fine slag in future.

关键词： Coal gasification Fine slag Multiscale analysis Carbon components Inorganic components

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Two UV organic-inorganic hybrid antimony-based materials with superior optical performance derived from cation-anion synergetic interactions

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Chinese Chemical Letters 2024年第9期35卷 442-446页

作者： Pu Zhang Xiang mao Xuehua Dong Ling huang Liling Cao Daojiang Gao Guohong Zou College of Chemistry and Materials Science Sichuan Normal UniversityChengdu 610066China College of Chemistry Sichuan UniversityChengdu 610065China

Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by ***,cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials,(C_(3)h_(5)N_(2))Sb F_(2)SO_(4)(I)and(C_(5)h_(6)N)Sb F_(2)SO_(4)(Ⅱ),which were obtained by introducing Sb^(3+)cation containing stereochemically active lone-pair(SCALP)and organicπ-conjugated cations into sulphate *** synergistic interactions of the organicπ-conjugated cations,the inorganic[SbO_(2)F_(2)]^(3-)seesaw anions and the[SO_(4)]^(2-)distorted tetrahedra anions make their ultraviolet(UV)absorption edges approach 297 and 283 nm,respectively,and raise their birefringence up to 0.193@546 nm and 0.179@546 nm,***,although the two compounds have the same stoichiometric ratio and similar one-dimensional(1D)chain structure,they show opposite macroscopic symmetry,where the NCS compound(Ⅱ)exhibits a large secondharmonic generation(ShG)response(1.6 times that of Kh_(2)PO_(4)).The two reported compounds are found to be promising UV optical materials in the experimental tests.

关键词： Antimony-based crystals Cation-anion synergetic interactions Large birefringence Short UV absorption edge Organic-inorganic hybrid Ionothermal synthesis

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Photocatalytic ozonation-based degradation of phenol by ZnO—TiO_(2)nanocomposites in spinning disk reactor

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Chinese Journal of Chemical Engineering 2024年第8期72卷 74-84页

作者： Xueqing Ren Jiahao Niu Yan Li Lei Li Chao Zhang qiang Guo Qiaoling Zhang Weizhou Jiao Shanxi Province Key Laboratory of higee-Oriented Chemical Engineering School of Chemistry and Chemical EngineeringNorth University of ChinaTaiyuan 030051China Shanxi Sanqiang New Energy Technology Co. LtdTaiyuan 030051China

Spinning disk reactor(SDR)has emerged as a novel process intensification photocatalytic reactor,and it has higher mass transfer efficiency and photon utilization for the degradation of toxic organic pollutants by advanced oxidation processes(AOPs).In this study,ZnO—TiO_(2)nanocomposites were prepared by solgel method,and coated on the disk of SDR by impregnation-pull-drying-calcination *** performance of catalyst was characterized by X-ray diffraction,scanning electron microscope,X-ray photoelectron spectroscopy,photoluminescence and ultraviolet—visible diffuse reflectance *** ozonation in SDR was used to remove phenol,and various factors on degradation effect were studied in *** results showed that the rate of degradation and mineralization reached 100%and 83.4%under UV light irradiation after 50 min,compared with photocatalysis and ozonation,the removal rate increased by 69.3%and 34.7%,and mineralization rate increased by 56.7%and 62.9%,which indicated that the coupling of photocatalysis and ozonation had a synergistic *** radical capture experiments demonstrated that the active species such as photogenerated holes(h^(+)),hydroxyl radicals(·Oh),superoxide radical(·O_(2)-)were responsible for phenol degradation,and·Oh played a leading role in the degradation process,while h+and·O_(2)^(-)played a non-leading role.

关键词： Spinning disk reactor Photocatalytic ozonation ZnO-TiO_(2)nanocomposites Advanced oxidation processes

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The photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(Oh)_(2)CO_(3)for stable photocatalytic CO_(2)reduction

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Journal of Energy Chemistry 2024年第5期92卷 104-112页

作者： Yaqing Zhi haoning mao Guangxing Yang Qiao Zhang Zhiting Liu Yonghai Cao Siyuan Yang Feng Peng School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006GuangdongChina College of Materials and Energy South China Agricultural UniversityGuangzhou 510642GuangdongChina School of Chemistry and Chemical Engineering South China University and TechnologyGangzhou 510640GuangdongChina

Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)***,monoclinic Cu_(2)(Oh)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and *** on a Cu_(2)(Oh)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(Oh)_(2)CO_(3)are definitely *** PCO_(2)R activity of Cu_(2)(Oh)_(2)CO_(3)is comparable to some of state-of-the-art novel ***,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(Oh)_(2)CO_(3)with typical TiO_(2)to construct composites *** highest CO_(2)and Ch_(4)production rates by 7.5 wt%Cu_(2)(Oh)_(2)CO_(3)-TiO_(2)reach.16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified *** work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.

关键词： CO_(2)photocatalytic reduction Photocatalysis Basic copper carbonate Self-reconstruction Photocatalyst

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Enhancing the electrocatalytic performance of nitrate reduction to ammonia by in-situ nitrogen leaching

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Chinese Chemical Letters 2024年第2期35卷 564-569页

作者： Mimi Fu Yini mao hua Wang Wei Luo Yimin Jiang Wei Shen Ming Li Rongxing he College of Chemistry and Chemical Engineering Southwest UniversityChongqing 400715China

Electrochemical nitrate reduction reaction (NITRR) is regarded as a “two birds-one stone” method for the treatment of nitrate contaminant in polluted water and the synthesis of valuable ammonia, which is retarded by the lack of highly reactive and selective electrocatalysts .herein, for the first time, nickel foam supported Co_(4) N was designed as a high-performance NITRR catalyst by an in-situ nonmetal leaching-induced *** the optimal potential, the Co_(4) N/NF catalyst achieves ultra-high Faraday efficiency and Nh_(3) selectivity of 95.4% and 99.4%, *** situ X-ray absorption spectroscopy (XAS), together with other experiments powerfully reveal that the nitrogen vacancies produced by nitrogen leaching are stable and play a key role in boosting nitrate reduction to *** calculations confirm that Co_(4) N with abundant nitrogen vacancies can optimize the adsorption energies of NO_(3)^(-) and intermediates, lower the free energy (Δ G ) of the potential-determining step (*Nh_(3) to Nh_(3) ) and inhibit the formation of N-containing *** addition, we also conclude that the nitrogen vacancies can stabilize the adsorbed hydrogen, making h_(2) quite difficult to produce, and lowering ΔG from *NO to *NOh, which facilitates the selective reduction of *** study reveals significant insights about the in-situ nonmetal leaching to enhance the NITRR activity.

关键词： Co4N Nitrate reduction In-situ nonmetal leaching Nitrogen vacancy Mechanism

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Recent advances in electrocatalytic generation of indole-derived radical cations and their applications in organic synthesis

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Chinese Chemical Letters 2024年第4期35卷 106-123页

作者： Wei Zhou Xi Chen Lin Lu Xian-Rong Song Mu-Jia Luo qiang Xiao Key Laboratory of Organic Chemistry of Jiangxi Province Jiangxi Science&Technology Normal UniversityNanchang 330013China

Indole-derived radical cations, open-shell reactive species, display distinctive dual reactivity due to the carbon-centered radical and more electrophilic carbocation, which frequently appear in a variety of single electron oxidation reactions for synthesizing structurally diverse functionalized indoles and indolines. Electrocatalysis is considered as a synthetically attractive and environmentally friendly alternative for driving the single electron oxidation of indoles. Remarkable achievements in electrocatalytic indolederived radical cation-mediated indole functionalization have been realized so far. This review comprehensively summarizes the recent progresses in the applications of electrocatalytic indole radical cations,including C(sp~2)–h functionalization, dearomative 2,3-difunctionalization, and ring-opening reaction, emphasizing the vital single electron oxidation steps of indoles, the substrates scope and limitations, and the reaction mechanisms.

关键词： Electrocatalysis Indole radical cation C-h functionalizatin Dearomative 2 3-difunctionalization

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∼2.5 nm pores in carbon-based cathode promise better zinc-iodine batteries

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Chinese Chemical Letters 2024年第5期35卷 471-476页

作者： Yajun hou Chuanzheng Zhu qiang Wang Xiaomeng Zhao Kun Luo Zongshuai Gong Zhihao Yuan School of Materials Science and Engineering Tianjin Key Laboratory of Photoelectric Materials&DevicesTianjin University of TechnologyTianjin 300384China

The relationship mechanism between the material pore structures and cathodic iodine chemistry plays a vital role in efficient Zn-I_(2) batteries,but is unclear,retarding further *** work innovatively indicates a great contribution of∼2.5nm pore structure of nanocarbons to efficient iodine adsorption,rapid I^(−)↔I_(2) conversion,and polyiodide inhibition,via scrupulously designing catalysts with controllable pore sizes *** I_(2)-loading within the designed nitrogen-doped nanocarbons can reach up to as high as 60.8 wt%.The batteries based on the cathode deliver impressive performances with a large capacity of 178.8 mAh/g and long-term cycling stability more than 4000 h at 5.0 ***,these is no polyiodide such as I_(3)−and I_(5)−detected during the charge-discharge processes from comprehensive electrochemical cyclic voltammetry,X-ray photoelectron spectroscopy,and Raman *** work provides a novel knowledge-guided concept for rational pore design,promising better Zn-I_(2) batteries,which is also hoped to benefit other advanced energy technologies,such as Li-S,Li-ion,and Al-I_(2) batteries.

关键词： Zinc-iodine batteries Structure-performance relationship Iodine conversion chemistry Cathode materials Porous carbon

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