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A new pathway for formic acid electro-oxidation:The electro-chemically decomposed hydrogen as a reaction intermediate

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Journal of Energy Chemistry 2022年第8期31卷 188-191,I0006页

作者： Xiaolong Yang Qinglei Meng Xian Wang Zhao Jin Changpeng Liu Junjie Ge Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 Jilin China School of Applied Chemistry and Engineering University of Science and Technology of China

Formic acid electro-oxidation reaction(FAOR)is generally believed that follows a two-pathway mechanism.Herein,we resorted to in situ electrochemical mass spectrometry and successfully captured the trace of H_(2),as the new intermediate species,during the process of FAOR on both Pt based catalyst and two single atom catalysts(Rh-N-C and Ir-N-C).Inspired by this,we proposed a new reaction path named hydrogen oxidation pathway:at the oxidation potential,formic acid will break the C–H bond and combine with the protons in the solution to form H_(2) species,then hydrogen oxidation reaction(HOR)will occur to generate two protons.This process is accompanied by electron transfer and contributes currently to the whole reaction.

关键词： Formic acid electro-oxidation reaction Hydrogen Pt Single atom catalysts reaction pathway

reaction pathway change on plasmonic Au nanoparticles studied by surface-enhanced Raman spectroscopy

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Chinese Chemical Letters 2021年第9期32卷 2846-2850页

作者： Ran Li Can-Can Zhang Dan Wang Yan-Fang Hu Yong-Long Li Wei Xie Key Lab of Advanced Energy Materials Chemistry(Ministry of Education) Tianjin Key Lab Mol Recognit&BiosensingRenewable Energy Conversion and Storage CenterCollege of ChemistryNankai UniversityTianjin 300071China

Gold nanoparticles(Au NPs)are nanoscale sources of light and electrons,which are highly relevant for their extensive applications in the field of photocatalysis.Although a number of research works have been carried out on chemical reactions accelerated by the energetic hot electrons/holes,the possibility of reaction pathway change on the plasmonic Au surfaces has not been reported so far.In this proof-ofconcept study,we find that Au NPs change the reaction pathway in photooxidation of alkyne under visible light irradiation.This reaction produces benzil(—CO—CO—)without the presence of Au NPs.In contrast,as indicated by surface-enhanced Raman spectroscopic(SERS)results,the C—C triple bonds(—C≡C—)adsorbed on Au NPs are converted into carboxyl(—COOH)and acyl chloride(—COCl)groups.The plasmonic Au NPs not only provide energetic charge carriers but also activate the reactant molecules as conventional heterogeneous catalysts.This study discloses the second role of plasmonic NPs in photocatalysis and bridges the gap between plasmon-driven and conventional heterogeneous catalysis.

关键词： Surface-enhanced Raman spectroscopy Surface plasmon Au nanoparticles Photocatalysis reaction pathway

Polyoxymethylene dimethyl ethers synthesis from methanol and formaldehyde solution over one-pot synthesized spherical mesoporous sulfated zirconia

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Chinese Journal of Chemical Engineering 2022年第6期35卷 161-172页

作者： Xiangjun Li Shujun Li Xiaoping Wang Muhammad Asif Nawaz Dianhua Liu State Key Lab of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

The synthesis of polyoxymethylene dimethyl ethers as an ideal diesel fuel additive is the current hot topic of modern petrochemical industry for their expedient properties in mitigating air pollutants emission during combustion.In this work,a series of spherical sulfated zirconia catalysts were prepared by a one-pot hydrothermal method assisted with surfactant cetyltrimethylammonium bromide(CTAB).The prepared sulfated zirconia catalysts were used to catalyze PODEn synthesis from methanol and formaldehyde solution.Various characterization(XRD,BET,SEM,TGA,NH_(3)-TPD,FTIR,and Py-IR)were employed to elaborate the structure–activity relationship of the studied catalytic system.The results demonstrated that S/Zr molar ratio in precursor solution played an effective role on catalyst morphology and acidic properties,where the weak Brønsted acid sites and strong Lewis acid sites were favorable to the conversion of methanol and formation of long-chain PODEn,respectively.The reaction parameters such as catalyst amount,molar ratio of FA/MeOH,reaction time,temperature and pressure were optimized.The speculated reaction pathway for PODEn synthesis was proposed based on the synergy of Brønsted and Lewis acid sites,which suggested that Brønsted and Lewis acid sites might be advantageous to the activation of polyoxymethylene hemiformals[CH_(3)(OCH_(2))_(n)OH]and methylene glycol(HOCH_(2)OH),respectively.

关键词： Polyoxymethylene dimethyl ethers Spherical sulfated zirconia Methanol Formaldehyde reaction pathway Synergistic effect

Effect of carbon dioxide on oxy-fuel combustion of hydrogen sulfide:An experimental and kinetic modeling

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中国化学工程学报:英文版 2023年第7期59卷 105-117页

作者： Xun Tao Fan Zhou Xinlei Yu Songling Guo Yunfei Gao Lu Ding Guangsuo Yu Zhenghua Dai Fuchen Wang Shanghai Engineering Research Center of Coal Gasification East China University of Science and TechnologyShanghai 200237China

CO_(2) is an important component in the acid gas and it is necessary to study the effect of CO_(2) presence on the oxy-fuel combustion of H_(2)S with particular focus on the formation of carbonyl sulfide(COS).The oxyfuel combustion of acid gas was conducted in a coaxial jet double channel burner.The distribution of flame temperature and products under stoichiometric condition along axial(R=0.0)and radial at about 3.0 mm(R=0.75)were analyzed,respectively.The Chemkin-Pro software was used to analyze the rate of production(ROP)for gas products and the reaction pathway of acid gas combustion.Both experimental and simulation results showed that acid gas combustion experienced the H2S chemical decomposition,H_(2)S oxidation and accompanied by H_(2) oxidation.The CO_(2) presence reduced the peak flame temperature and triggered the formation of COS in the flame area.COS formation at R=0.0 was mainly through the reaction of CO_(2) and CO with sulfur species,whereas at R=0.75 it was through the reaction of CO with sulfur species.The ROP results indicated that H_(2) was mainly from H_(2)O decomposition in the H_(2)S oxidation stage,and COS was formed by the reaction of CO_(2) with H_(2)S.ROP and other detailed analysis further revealed the role of H,OH and SH radicals in each stage of H_(2)S conversion.This study revealed the COS formation mechanisms with CO_(2) presence in the oxy-fuel combustion of H_(2)S and could offer important insights for pollutant control.

关键词： Carbon dioxide Oxy-fuel combustion of H_(2)S reaction pathway Kinetics Oxidation

Electrochemical Biorefinery toward Chemicals Synthesis and Bio-Oil Upgrading from Lignin

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Engineering 2023年第8期27卷 178-198页

作者： Rui Hu Yuying Zhao Chen Tang Yan Shi Gang Luo Jiajun Fan James H.Clark Shicheng Zhang Shanghai Technical Service Platform for Pollution Control and Resource Utilization of Organic Wastes Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3)Department of Environmental Science and EngineeringFudan UniversityShanghai 200438China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Circa Renewable Chemistry Institute Green Chemistry Center of ExcellenceDepartment of ChemistryUniversity of YorkYork YO105DDUK

Recalcitrance and the inherent heterogeneity of lignin structure are the major bottlenecks to impede the popularization of lignin-based chemicals production processes.Recent works suggested a promising pathway for lignin depolymerization and lignin-derived bio-oil upgrading via an electrochemical biorefinery(a process in which lignin valorization is performed via electrochemical oxidation or reduction).This review presents the progress on chemicals synthesis and bio-oil upgrading from lignin by an electrochemical biorefinery,relating to the lignin biosynthesis pathway,reaction pathway of lignin electrochemical conversion,inner-sphere and outer-sphere electron transfer mechanism,basic kinetics and thermodynamics in electrochemistry,and the recent embodiments analysis with the emphasis on the respective feature and limitation for lignin electrochemical oxidative and reductive conversion.Lastly,the challenge and perspective associated with lignin electrochemical biorefinery are discussed.Present-day results indicate that more work should be performed to promote efficiency,selectivity,and stability in pursuing a lignin electrochemical biorefinery.One of the most promising developing directions appears to be integrating various types of lignin electrochemical conversion strategies and other existing or evolving lignin valorization technologies.This review aims to provide more references and discussion on the development for lignin electrochemical biorefinery.

关键词： Lignin Electrochemical biorefinery reaction pathway Electron transfer mechanism Kinetics Thermodynamics

Au core-PtAu alloy shell nanowires for formic acid electrolysis

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Journal of Energy Chemistry 2022年第2期31卷 94-102页

作者： Qi Xue Xin-Yu Bai Yue Zhao Ya-Nan Li Tian-Jiao Wang Hui-Ying Sun Fu-Min Li Pei Chen Pujun Jin Shi-Bin Yin Yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(MOE)Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710062ShaanxiChina MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsGuangxi UniversityNanning 530004GuangxiChina

Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water electrolysis.Herein we report the one-pot precise synthesis of ultrafine Au core-Pt Au alloy shell nanowires(Au@PtxAu UFNWs).Among them,Au@Pt_(0.077) Au UFNWs exhibit the best performance for formic acid oxidation reaction(FAOR)and hydrogen evolution reaction(HER),which only require applied potentials of 0.29 V and-22.6 m V to achieve a current density of 10 m A cm^(-2),respectively.The corresponding formic acid electrolyzer realizes the electrochemical H2 production at a voltage of only 0.51 V with 10 m A cm^(-2) current density.Density functional theory(DFT)calculations reveal that the Au-riched Pt Au alloy structure can facilitates the direct oxidation pathway of FAOR and consequently elevates the FAOR activity of Au@Pt_(0.077) Au UFNWs.This work provides meaningful insights into the electrochemical H_(2) production from both the construction of advanced bifunctional electrocatalysts and the replacement of OER.

关键词： Au core-PtAu alloy shell nanowires Formic acid oxidation reaction reaction pathway Hydrogen evolution reaction Acidic water electrolysis

Earth-Abundant CaCO_(3)-Based Photocatalyst for Enhanced ROS Production,Toxic By-Product Suppression,and Efficient NO Removal

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Energy & Environmental Materials 2022年第3期5卷 928-934页

作者： Wen Cui Wenjia Yang Peng Chen Lvcun Chen Jieyuan Li Yanjuan Sun Ying Zhou Fan Dong The Center of New Energy Materials and Technology School of Materials Science and EngineeringSouthwest Petroleum UniversityChengdu 610500China Yangtze Delta Region Institute(Huzhou)&Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaHuzhou 313000China Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and ResourcesChongqing Technology and Business UniversityChongqing 400067China State Centre for International Cooperation on Designer Low Carbon and Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China

Photoinduced reactive oxygen species(ROS)-based pollutant removal is one of the ideal solutions to achieve the conversion of solar energy into chemical energy and thus to address environmental pollution.Here,earthabundant CaCO_(3)-decorated g-C_(3)N_(4)(g-C_(3)N_(4)labeled as CN,CaCO_(3)-decorated g-C_(3)N_(4)sample labeled as CN-CCO)has been constructed by a facile thermal polymerization method for safe and efficient photocatalytic NO removal.The decorated CaCO_(3)as“transit hub”extends theπbonds of CN to deviate from the planes and steers the random charge carriers,which thus provides extra active sites and expedites spatial charge separation to facilitate adsorption/activation of reactants and promote formation of ROS participating in the removal of pollutant.Furthermore,boosted generation of ROS regulates the photocatalytic NO oxidation pathway and thus increases the selectivity of products.NO prefers to be directly oxidized into final product(nitrate)rather than toxic intermediates(NO_(2)),which is well demonstrated by theoretically simulated ROS-based reaction pathways and experimental characterization.The present work promotes the degradation of pollutant and simultaneously suppresses the formation of toxic by-product,which paves the way for ROS-based pollutant removal.

关键词： in situ DRIFTS photocatalytic NO removal reaction pathway ROS production toxic by-product suppression

Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1700-1712页

作者： Dongyang Liu Yibo Zhi Yuen Bai Liang Zhao Jinsen Gao Chunming Xu State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249China

The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha.Herein,for a better catalyst design and operation parameters optimization,the reaction pathways and equilibrium yields for the catalytic pyrolysis of C_(5-8)n/iso/cyclo-paraffins were analyzed thermodynamically.The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways,respectively.However,the formation of light paraffin severely limits the maximum selectivity toward light olefins.The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins.The results are thus useful as a direction for future catalyst improvements,facilitating superior reaction pathways to enhance light olefins.In addition,the equilibrium yield of light olefins increased with increasing the chain length,and the introduction of cyclo-paraffin inhibits the formation of light olefins.High temperatures and low pressures favor the formation of ethylene,and moderate temperatures and low pressures favor the formation of propylene.n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90%and 55.77%,respectively.This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C_(5-8)n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha catalytic pyrolysis reaction pathway equilibrium yield

Pt-Te alloy nanowires towards formic acid electrooxidation reaction

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Journal of Energy Chemistry 2023年第10期85卷 481-489,I0013页

作者： Bin Sun Yu-Chuan Jiang Qing-Ling Hong Xue Liu Fu-Min Li Dong-Sheng Li Yun Yang Yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province School of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710062ShaanxiChina Nanomaterials and Chemistry Key Laboratory Wenzhou UniversityWenzhou 325035ZhejiangChina School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074HubeiChina College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002HubeiChina

The high-performance anodic electrocatalysts is pivotal for realizing the commercial application of the direct formic acid fuel cells.In this work,a simple polyethyleneimine-assisted galvanic replacement reaction is applied to synthesize the high-quality PtTe alloy nanowires(PtTe NW)by using Te NW as an efficient sacrificial template.The existence of Te atoms separates the continuous Pt atoms,triggering a direct reaction pathway of formic acid electrooxidation reaction(FAEOR)at PtTe NW.The one-dimensional architecture and highly active sites have enabled PtTe NW to reveal outstanding electrocatalytic activity towards FAEOR with the mass/specific activities of 1091.25 mA mg^(-1)/45.34 A m^(-2)at 0.643 V potential,which are 44.72/23.16 and 20.26/11.75 times bigger than those of the commercial Pt and Pd nanoparticles,respectively.Density functional theory calculations reveal that Te atoms optimize the electronic structure of Pt atoms,which decreases the adsorption capacity of CO intermediate and simultaneously improves the durability of PtTe NW towards FAEOR.This work provides the valuable insights into the synthesis and design of efficient Pt-based alloy FAEOR electrocatalysts.

关键词： Formic acid electrooxidation PtTe alloy nanowires Galvanic replacement reaction reaction pathway Fuel cells