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Highly efficient photo-thermal synergistic catalysis of CO_(2)methanation over La_(1-x)Ce_(x)NiO_(3)perovskite-catalyst

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Nano Research 2024年第9期17卷 7945-7956页

作者： Ting Li Zhen-Yu Zhang De-Cun Luo Bo-Yu Xu Rong-Jiang Zhang Ji-Long Yao Dan Li Tao Xie Institute of Industrial Catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

Solar-driven photo-thermal catalytic CO_(2)methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases ***,designing advanced photo-thermal catalysts remains a research challenge for CO_(2)methanation *** this work,a series of ABO3(A=lanthanide,B=transition metal)perovskite catalysts with Ce-substituted LaNiO3(La_(1-x)Ce_(x)NiO_(3),x=0,0.2,0.5,0.8,1)were synthesized for CO_(2)*** La_(0.2)Ce_(0.8)NiO_(3) exhibited the highest CH_(4) formation rate of 258.9 mmol·g^(-1)·hcat-1,CO_(2)conversion of 55.4%and 97.2%CH_(4) selectivity at 300℃with the light intensity of 2.9 W·cm^(-2).Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties *** partial substitution of the A-site provided more active sites for the adsorption and activation of CO_(2)/H_(2).The sources of the active sites were considered to be the oxygen vacancies(O_(v))created by lattice distortions due to different species of ions(La^(3+),Ce^(4+),Ce^(3+))and exsolved Ni0 by H_(2)*** catalysts have excellent light absorption absorbance and low electron-hole(e^(-)/h^(+))recombination rate,which greatly contribute to the excellent performance in photo-thermal synergistic catalysis(PTC)CO_(2)*** results of in situ irradiated electron paramagnetic resonance spectrometer(ISI-EPR)and ISI-X-ray photoelectron spectroscopy(XPS)indicated that the aggregation of unpaired electrons near the defects and Ni metal(from La and Ce ions to Ov and Ni0)accelerated adsorption and activation of CO_(2)/H_(2).At last,the catalyst properties and structure were correlated with the proposed reaction mechanism from the in situ diffuse reflection infrared Fourier transform spectrum(DRIFTS)*** in situ precipitation of the B-site enhanced the dispersion of Ni,while its enriched photoelectrons upon illumination further promote hydrogen *** H^(*)spillover accelerated t

关键词： photo-thermal catalysis CO_(2)methanation perovskite A-site substitution in situ diffuse reflection infrared Fourier transform spectrum(DRIFTS)

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Progress on gas-solid phase photoreactor and its application in CO_(2) reduction

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Green chemical Engineering 2024年第3期5卷 290-306页

作者： Litian Liu Yunlong Li Jialun He Qing Wang Juan Deng Xiao Chen Chao Yu school of Environmental and chemical Engineering Jiangsu University of Science and TechnologyZhenjiang212100China

The burgeoning field of photocatalytic reduction of CO_(2)has emerged as a remarkable promising solution to address some of the most pressing global energy and environmental issues which we face *** around the global have been striving to augment the efficiency of CO_(2)photocatalytic reduction,employing strategies that range from modifying the fundamental properties of photocatalysts to suppress the electron-hole recombination,optimizing reaction conditions to achieve the highest yield,and conceptualizing and constructing photoreactors to improve the adsorption *** these factors,the photoreactor plays a critical role in enhancing the overall photocatalytic *** the various types of photoreactors and their operational dynamic can significantly influence the experimental design,thus guiding the data collecting and *** to the solid-liquid phase,gas-solid phase photocatalytic reduction of CO_(2)is gaining recognition for its potential advantages,such as rapid molecular diffusion rates,adjustable CO_(2)concentrations,and uniform and sufficient light ***,the currently reported gas-solid phase photoreactors are still in their *** this review,we dissect the underlying mechanism of photocatalytic CO_(2)reduction and the performance evaluation criteria of photoreactors,and review the development process of gas-solid phase ***,we explore the evolution of gas-solid phase photoreactors,elucidating their growth trajectory and future *** present a comprehensive classification of gas-solid phase photoreactors,offering a new insight into their design and functionality,summarizing their strengths and inevitable ***,we provide a forward-looking perspective on the future developmental prospects of carbon neutrality.

关键词： Photoreactor Gas-solid phase Carbon dioxide reduction Photocatalysis

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RuO_(2)/CoMO_(2)O_(x) Catalyst with Low Ruthenium Loading for Long-Term Acidic Oxygen Evolution

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Transactions of Tianjin University 2024年第5期30卷 395-405页

作者： Yingying Wang Hui Pan Zhikun Liu Peng Kang school of chemical Engineering and Technology Tianjin UniversityTianjin 300072China

We must urgently synthesize highly efficient and stable oxygen-evolution reaction(OER) catalysts for acidic media. Herein, we constructed a series of Ti mesh(TM)-supported RuO_(2)/CoMo_(y)O_(x) catalysts(RuO_(2)/CoMo_(y)O_(x)/TM) with heterogeneous structures. By optimizing the ratio of Co to Mo, RuO_(2)/CoMO_(2)O_(x)/TM with low Ru loading(0.079 mg/cm^(2)) achieves remarkable OER performance(η = 243 mV at 10 mA/cm^(2)) and high stability(300 h @ 10 mA/cm^(2)) in 0.5 mol/L H_(2)SO_(4) electrolyte. The activity of RuO_(2)/CoMo_yO_x/TM can be maintained for 50 h at 100 mA/cm^(2), and a water electrolyzer with RuO_(2)/CoMO_(2)O_(x)/TM as anode can operate for 40 h at 100 mA/cm~2, suggesting the remarkable OER durability of RuO_(2)/CoMo__(y)O__(x)/TM in acidic electrolyte. Owing to the heterogeneous interface between CoMO_(2)O_(x) and RuO_(2), the electronic structure of Ru atoms was optimized and electron-rich Ru was formed. With modulated electronic properties, the dissociation energy of H_(2)O is weakened, and the OER barrier is lowered. This study provides the design of low-cost noble metal catalysts with long-term stability in an acidic environment.

关键词： Oxygen-evolution reaction Ru-based catalyst Acidic media Heterostructure Long-term electrolysis Low precious metal

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Controllable Construction of Vinyl Sulfones and β-Keto Selenosulfones via Selective Oxidative Sulfonylation of Alkenes

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Chinese Journal of Chemistry 2024年第12期42卷 1367-1372页

作者： Xiang Liu Yuan Zhang Yi Zheng Changfeng Huang Hua Cao school of Chemistry and chemical Engineering Guangdong Pharmaceutical UniversityZhongshanGuangdong 528458China

Comprehensive Summary The selective oxidative sulfonylation of alkenes with selenium sulfonate depended on the reaction *** electrochemical C—H sulfonylation proceeded smoothly to afford(E)-vinyl sulfones with good selectivity in an undivided cell without external *** aerobic trifunctionalization of alkenes occurred in the presence of KI in the air,which providesβ-keto selenosulfones via the formation of C—O,C—S,and C—Se bonds in *** control experiments,a plausible mechanism is proposed to rationalize the experimental results.

关键词： Synthetic methods Alkenes Difunctionalization Selenylation Sulfonylation

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Sustainable and practical semi-heterogeneous photosynthesis of 5-amino-1,2,4-thiadiazoles over WS_(2)/TEMPO

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Chinese chemical Letters 2024年第8期35卷 250-253页

作者： Jia-Cheng Hou Hong-Tao Ji Yu-Han Lu Jia-Sheng Wang Yao-Dan Xu Yan-Yan Zeng Wei-Min He school of Chemistry and chemical Engineering University of South ChinaHengyang 421001China

An eco-friendly and practical method for the clean preparation of 5-amino-1,2,4-thiadiazoles was *** WS_(2)as the semiconductor photocatalyst,both TEMPO and O_(2)(in air)as the redox catalysts,a variety of thiadiazoles were semi-heterogeneously formed in high to quantitative yields and could be easily collected by CPME extraction and ***,the catalytic system can be reusable for at least 5 reaction runs.

关键词： Green chemistry Thiadiazoles Heterogeneous catalyst Redox catalyst Extraction

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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of Energy Chemistry 2024年第8期95卷 20-28,I0002页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key Lab of Fine chemicals Liaoning Key Lab for Energy Materials and Chemical EngineeringFrontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Liaoning Key Lab for Energy Materials and chemical Engineering Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon ***,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging ***,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center *** experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-π*** multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive *** defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the *** work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Defect engineering Pentagon carbon Carbon quantum dots Electrocatalytic activity Triiodide reduction

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Construction of pyrene-based hydrogen-bonded organic frameworks as photocatalysts for photooxidation of styrene in water

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Chinese chemical Letters 2024年第10期35卷 394-398页

作者： Rongxin Zhu Shengsheng Yu Xuanzong Yang Ruyu Zhu Hui Liu Kaikai Niu Lingbao Xing school of Chemistry and chemical Engineering Shandong University of TechnologyZibo 255000China

Using hydrogen-bonded organic frameworks(HOFs)as photosensitizers to perform photocatalytic oxidation reactions under green and mild conditions is still a challenge for the application of HOFs *** study presents a novel approach that exploits HOFs to enhance the efficiency of photocatalytic oxidation for achieving visible light catalytic oxidation of styrene and its derivatives in the aqueous *** using 1,3,6,8-tetrakis(p-benzoic acid)pyrene(H_(4)TBAPy)as the monomer,a pyrene-based hydrogen-bonded organic framework(PFC-1)with a microporous structure was successfully *** with monomer H_(4)TBAPy,due to the exciton effect and the interlayer confinement of HOFs,the singlet oxygen(1O_(2))production efficiency is significantly improved,which has great potential in photocatalytic oxidation ***,the practicality of PFC-1 as a photocatalyst was studied,and the photocatalytic oxidation of styrene and its derivatives in aqueous solution was achieved under visible light with high catalytic efficiency,indicating that PFC-1 has significant potential to promote photocatalytic oxidation reactions under mild *** utilization of HOFs as photosensitizers in this straightforward approach enables the attainment of green photocatalytic oxidation,hence expanding the potential applications of HOFs materials within the realm of photocatalysis.

关键词： Pyrene Hydrogen-bonded organicframeworks Singlet oxygen Photocatalysis Styrene

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MnO-pillared graphene blocks enabling the ultrastable and ultrafast aqueous zinc ion batteries

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Science China Chemistry 2024年第9期67卷 2930-2940页

作者： Zheng Liu Zhipeng Qiu Zhiyuan Li Tong Wei Zhuangjun Fan Huan Pang school of Chemistry and chemical Engineering Yangzhou UniversityYangzhou 225002China school of Materials Science and Engineering China University of PetroleumQingdao 266580China

Due to the low cost,high theoretical capacity,and environmental friendliness,manganese-based cathodes are regarded as promising alternatives for aqueous zinc ion batteries(AZIBs).However,the practicality of the zinc-manganese system is faced with great challenges,such as the inevitable structural collapse of the cathode and controversial energy storage ***,we propose a novel concept of spatial deposition mechanism through the addition of MnSO_(4) additives in the Mn O-pillared graphene blocks(G-MnO).The covalent interface between MnO nanoparticles and multilayered graphene nanosheets can construct an in-built micro-electric field,which is beneficial for consecutive electron transfer(in both horizontal and vertical directions).On this basis,the surficial activity of MnO confined in the interlayered nano-space is greatly enhanced and provides enough spatial deposition and subsequent reaction site for MnSO_(4) additives,thus firstly extending the surficial controlled process to stereoscopic space,effectively improving the electrochemical performance of ***,the assembled Zn//G-Mn O battery exhibits an excellent rate capability of 281.5 mAhg^(-1)at 0.1 A g^(-1)and 106 mAhg^(-1)at 20 Ag^(-1),and impressive cycling stability(93 mAhg^(-1)remaining after 5,000 cycles).This finding may provide a new opportunity for the rational design of surficial controlled energy storage and conversion devices.

关键词： zinc-ion battery manganese monoxide laminated constructure ultrahigh rate performance graphene

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An effective'salt in dimethyl sulfoxide/water'electrolyte enables high-voltage supercapacitor operated at-50℃

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Journal of Energy Chemistry 2024年第6期93卷 361-367,I0009页

作者： Yingbin Liu Chang Yu Xuedan Song Siyi Hou Shuqin Lan Jinhe Yu Yuanyang Xie Jieshan Qiu State Key Lab of Fine chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina school of Chemistry Frontier Science Center for Smart MaterialsLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in ***,challenges remain for low-salt aqueous electrolytes operating at high voltage and low ***,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid ***,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid *** paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 *** modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.

关键词： Dimethyl sulfoxide Co-solvent High voltage Low temperature Supercapacitors

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Preparation and Characterization of Biobased Dehydroabietyl Polyethylene Glycol Glycidyl Ether-Grafted Hydroxyethyl Cellulose with High Emulsifying Property

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Journal of Renewable Materials 2024年第1期12卷 103-117页

作者： Zhengqing Ding Quan Yang Xinyan Yan Feng Gu Xujuan Huang Zhaosheng Cai school of chemical and Chemistry Yancheng Institute of TechnologyYancheng224051China

Dehydroabietyl polyethylene glycol glycidyl ether-grafted hydroxyethyl cellulose(HEC)polymer surfactant(DA(EO)5GE-g-HEC)was prepared using ring-opening polymerization with biobased rosin and hydroxyethyl cellulose as *** polyethylene glycol glycidyl ether(DA(EO)5GE)was formed by condensation of dehydroabietyl alcohol polyoxyethylene ether(Rosin derivative:DA(EO)5H)and *** grafting degree of DA(EO)5GE-g-HEC was manipulated by adjusting the mass ratio of HEC and DA(EO)5GE and confirmed by *** to the formula,when m(HEC)/m(DA(EO)2GE)was 1:1~1:5,the grafting rate of DA(EO)5GE in DA(EO)5GE-g-HEC varied from 34.43%to 38.33%.The surface activity and foam properties of DA(EO)5GE-g-HEC aqueous solution were *** results showed that with the increase in grafting rate,the critical micellar concentration(CMC)in aqueous solution changed from 1.28 to 0.96 g/*** results of the thermogravimetric analysis showed that the temperature range of the main stage of mass loss of DA(EO)5GE-g-HEC was 310°C~410°C,and the thermal decomposition processes of the samples with five mass ratios were *** oil in water emulsion was prepared by choosing cyclohexane as the oil phase and DA(EO)5GE-g-HEC as the *** effect of DA(EO)5GE-g-HEC mass fraction on emulsion particle size and stability was *** results suggested that when the oil-water ratio was 8:2 with 0.4%emulsifier,the emulsion droplets were the smallest in terms of particle size and were the most *** rheological test results showed that the apparent viscosity decreased with the increase in shear rate and showed a typical elastic gel phenomenon.

关键词： Rosin hydroxyethyl cellulose surfactant emulsion rheological behaviour

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