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Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song State key laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)*** herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) *** surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) *** example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V ***,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl *** virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and *** this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed *** work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

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Apically guiding electron/mass transfer reaction induced by Ag/FeN_(x)Mott-Schottky effect within a hollow star reactor toward high performance zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 106-116,I0004页

作者： Kaixiang Shi Kaixin Wang Tong Li Junhao Li Jie Ren Xu Li Yonggang Min Zhouguang Lu Wei Tan Quanbing Liu guangdong Provincial laboratory of Chemistry and Fine Chemical Engineering Jieyang Center(Rongjiang laboratory) Guangdong University of TechnologyJieyang 515200GuangdongChina Guangzhou key laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources BiorefinerySchool of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006GuangdongChina key laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan province School of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou 571158HainanChina School of Materials and Energy Guangdong University of TechnologyGuangzhou 510006GuangdongChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055GuangdongChina

The disparity in the transfer of carriers(electrons/mass)during the reaction in zinc-air batteries(ZABs)results in sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),along with elevated overpotentials,thereby imposing additional constraints on its ***,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently *** this work,an apically guiding dual-functional electrocatalyst(Ag-FeN_(x)-N-C)was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional(3D)hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride(FeN_(x))*** calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeN_(x),of which electron accumulation in the FeN_(x)phase region and electron depletion in the Ag phase region promote orientated-guiding charge *** effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/***,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass *** results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm^(-2).A rechargeable ZAB with Ag-FeN_(x)-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles(500 h),with a power density of 180 mW cm^(-2).Moreover,when employing AgFeN_(x)-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm^(-2).Ag-FeN_(x)-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the explo

关键词： Hollow star structure Mott-Schottky effect Apically guiding effect Bifunctional catalysis Zinc-air batteries

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Introducing sulfur to nickel-iron selenide for high-efficiency alkaline seawater electrolysis

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Science China Chemistry 2024年第8期67卷 2747-2754页

作者： Xuanwa Chen Yanhui Yu Xingqi Han Huan Wang Yingjie Hua Daoxiong Wu Peilin Deng Juanxiu Xiao Xinlong Tian Jing Li School of Marine Science and Engineering Hainan Provincial Key Lab of Fine ChemistrySchool of Chemistry and Chemical EngineeringHainan UniversityHaikou 570228China key laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China key laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan province School of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou 571158China

Seawater electrolysis is an effective way to obtain hydrogen(H_(2))in a sustainable ***,the lack of electrocatalysts with high activity,stability,and selectivity for oxygen evolution reaction(OER)severely hinders the development of seawater electrolysis ***,sulfur-doped nickel-iron selenide nanosheets(S-NiFeSe_(2))were prepared by an ion-exchange strategy and served as highly active OER electrocatalyst for alkaline seawater *** overpotential is 367 m V,and it can run stably for over 50 h at 100 m A cm^(-2).Excitingly,the S-NiFeSe_(2)||Pt/C pair exhibits cell voltage of 1.54 V at 10 m A cm^(-2)under alkaline seawater conditions,which can run smoothly for 100 h without decay,and the efficiency of electricity-tohydrogen(ETH)energy conversion reaches more than 80%.Such electrode,with abundant accessible reactive sites and good corrosion resistance,is a good candidate for seawater ***,density functional theory calculations reveal that the surface sulfur atoms can activate the adjacent Ni sites and decrease the free energy changes of the associated intermediates at the adjacent Ni sites for OER,and the step of~*OH→~*O is the potential rate-limiting *** this work,the true reactive site in nickel-iron selenides is the Ni sites,but not the Fe sites as commonly believed.

关键词： S-doping nickel-iron selenide electrocatalysts oxygen evolution reaction alkaline seawater electrolysis

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Effect of Different Calcination Temperatures on the Structure and Properties of Zirconium-Based Coating Layer Modified Cathode Material Li_(1.2)Mn_(0.54)Ni_(0.13)Co_(0.13)O_(2)

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Acta Metallurgica Sinica(English Letters) 2022年第6期35卷 985-995页

作者： Zijun Liao Jiankai Kang Qi Luo Caifeng Pan Jiangdong Chen Xiaolong Mo Hanbo Zou Wei Yang Shengzhou Chen School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006China Institute of Energy and Catalysis Guangzhou UniversityGuangzhou 510006China key laboratory of fuel cell technology of guangdong province Guangzhou 510006China

Lithium-rich manganese-based oxides have the advantages of high discharge specific capacity, so they are potential candidates for advanced lithium battery cathode materials. However, they also have drawbacks to be solved such as serious irreversible loss of capacity and voltage decay in the cycling process. Surface coating method was used in this paper to modify the lithium-rich manganese-based oxide(LRMO,Li_(1.2)Mn_(0.54)Ni_(0.13)Co_(0.13)O_(2)) to improve its electrochemical properties. Zirconium-based compounds coated LRMO materials(ZBC@LRMO) were obtained via the reaction of lithium hydroxide with zirconium n-butanol and subsequent thermal treatment at different temperatures. The results of X-ray diffraction and transmission electron microscopy confirm that the crystal structure and composition of the ZBC coating layer vary with the calcination temperature. The coating layer obtained at 600 ℃ is composed of tetragonal ZrO_(2) and Li_(2)ZrO_(3). The ZBC@LRMO sample with tetragonal ZrO =2 and Li_(2)ZrO_(3) composite exhibits the best electrochemical performance: the discharge capacity of ZBC@LRMO can reach 296 mAh g^(-1) at 0.1 C and 120 mAh g^(-1) at high rate of 5 C.

关键词： Lithium-ion battery Cathode material Zirconium-based compounds coating Calcination temperature Electrochemical performance

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Renewable wood-derived hierarchical porous,N-doped carbon sheet as a robust self-supporting cathodic electrode for zinc-air batteries

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Chinese Chemical Letters 2023年第1期34卷 133-138页

作者： Xiaohua Deng Zhu Jiang Yingying Chen Dai Dang Quanbing Liu Xiaoyang Wang Xu Yang School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Department of Chemical Systems Engineering Graduate School of EngineeringNagoya UniversityFuro-choChikusa-kuNagoya 464-8603Japan

Heteroatom doped porous carbon materials have emerged as essential cathode material for metal-air battery systems in the context of soaring demands for clean energy conversion and ***,a three-dimensional nitrogen-doped carbon self-supported electrode(TNCSE)is fabricated through thermal treatment and acid activation of raw *** resulting TNCSE retains the hierarchical porous architecture of parent raw lumber and holds substantial defect sites and doped N sites in the carbon *** as a cathode in the rechargeable zinc-air battery,the TNCSE exhibits a superior peak power density of 134.02 m W/cm^(2)and an energy density of 835.92 m Ah/g,significantly exceeding the ones reference commercial 20%Pt/C *** strikingly,a limited performance decay of 1.47%after an ultra long-period(500 h)cycle is also achieved on the *** work could offer a green and cost-save approach for rationally converting biomass into a robust self-supporting cathode material for a rechargeable zinc-air battery.

关键词： Carbon sheet Hierarchical porous structure Metal-free Zinc-air batteries Long-life stability

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Enabling high-efficiency ethanol oxidation on NiFe-LDH via deprotonation promotion and absorption inhibition

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Journal of Energy Chemistry 2023年第10期85卷 76-82,I0004页

作者： Jiawei Shi Huawei He Yinghua Guo Feng Ji Jing Li Yi Zhang Chengwei Deng Liyuan Fan Weiwei Cai Hydrogen Energy technology Innovation Center of Hubei province Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074HubeiChina State key laboratory of Space Power-Sources technology Shanghai Institute of Space Power SourcesShanghai 200245China College of Science and Engineering James Cook University1 James Cook DriveTownsvilleQLD 4811Australia

Nucleophile oxidation reaction(NOR), represented by ethanol oxidation reaction(EOR), is a promising pathway to replace oxygen evolution reaction(OER). EOR can effectively reduce the driving voltage of hydrogen production in direct water splitting. In this work, large current and high efficiency of EOR on a Ni, Fe layered double hydroxide(NiFe-LDH) catalyst were simultaneously achieved by a facile fluorination strategy. F in NiFe-LDH can reduce the activation energy of the dehydrogenation reaction, thus promoting the deprotonation process of NiFe-LDH to achieve a lower EOR onset potential. It also weakens the absorption of OH-and nucleophile electrooxidation products on the surface of NiFe-LDH at a higher potential, achieving a high current density and EOR selectivity, according to density functional theory calculations. Based on our experiment results, the optimized fluorinated NiFe-LDH catalyst achieves a low potential of 1.386 V to deliver a 10 mA cm^(-2)EOR. Moreover, the Faraday efficiency is greater than 95%, with a current density ranging from 10 to 250 mA cm^(-2). This work provides a promising pathway for an efficient and cost-effective NOR catalyst design for economic hydrogen production.

关键词： Ethanol oxidation reaction High efficiency Ni Fe layered double hydroxide Fluorination strategy Deprotonation

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Interface Engineering of NixSy@MnOxHy Nanorods to Efficiently Enhance Overall-Water-Splitting Activity and Stability

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Nano-Micro Letters 2022年第7期14卷 246-262页

作者： Pan Wang Yuanzhi Luo Gaixia Zhang Zhangsen Chen Hariprasad Ranganathan Shuhui Sun Zhicong Shi Institute of Batteries School of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006People’s Republic of China Énergie Matériaux Télécommunications research Centre Institut National de La Recherche Scientifique(INRS)VarennesQuébec J3X 1P7Canada The key laboratory of fuel cell technology of guangdong province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641People’s Republic of China

Exploring highly active and stable transition metal-based bifunctional electrocatalysts has recently attracted extensive research interests for achieving high inherent activity, abundant exposed active sites, rapid mass transfer, and strong structure stability for overall water splitting. Herein, an interface engineering coupled with shell-protection strategy was applied to construct three-dimensional(3D) core-shell NixSy@MnOxHy heterostructure nanorods grown on nickel foam(NixSy@MnOxHy/NF) as a bifunctional electrocatalyst. NixSy@MnOxHy/NF was synthesized via a facile hydrothermal reaction followed by an electrodeposition process. The X-ray absorption fine structure spectra reveal that abundant Mn-S bonds connect the heterostructure interfaces of N ixSy@MnOxHy, leading to a strong electronic interaction, which improves the intrinsic activities of hydrogen evolution reaction and oxygen evolution reaction(OER). Besides, as an efficient protective shell, the MnOxHy dramatically inhibits the electrochemical corrosion of the electrocatalyst at high current densities, which remarkably enhances the stability at high potentials. Furthermore, the 3D nanorod structure not only exposes enriched active sites, but also accelerates the electrolyte diffusion and bubble desorption. Therefore, NixSy@MnOxHy/NF exhibits exceptional bifunctional activity and stability for overall water splitting, with low overpotentials of 326 and 356 mV for OER at 100 and 500 mA cm^(–2), respectively, along with high stability of 150 h at 100 mA cm^(–2). Furthermore, for overall water splitting, it presents a low cell voltage of 1.529 V at 10 mA cm^(–2), accompanied by excellent stability at 100 mA cm^(–2) for 100 h. This work sheds a light on exploring highly active and stable bifunctional electrocatalysts by the interface engineering coupled with shell-protection strategy.

关键词： Interface engineering Protective shell Manganese compound Nickel sulfides Bifunctional Water splitting

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Rational design ternary platinum based electrocatalysts for effective methanol oxidation reaction

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Journal of Energy Chemistry 2022年第7期31卷 230-235,I0007页

作者： Hao Tian Daoxiong Wu Jing Li Junming Luo Chunman Jia Zhongxin Liu Wei Huang Qi Chen Chong Michael Shim Peilin Deng Yijun Shen Xinlong Tian State key laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228HainanChina

Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,and expandable method is developed to synthesis two-dimensional(2D) ternary Pt Bi M nanoplates(NPLs), in which various M(Co, Ni, Cu, Zn, Sn) is severed as the third component to the binary Pt Bi system. The MOR performance of Pt Bi M NPLs is entirely investigated, demonstrating that both the MOR activity and durability is enhanced with the introduction of the additional composition. Pt3Bi3Zn NPLs shows much higher MOR activity and stability than that of the Pt Bi counterparts, not to mention the current advanced Pt Ru/C and Pt/C catalysts. The prominent performances are attributed to the modulated electronic structure of the surface Pt in Pt Bi NPLs by the addition of Zn, resulting in a weakened affination between Pt and the adsorbed poisoning species(mainly CO) compared with Pt Bi NPLs, verified by density functional theory(DFT) calculations. In addition, the absorbed OH can be generated on the surface of Zn atom due to its favorable water activation properties, thus the CO removal on the adjacent Pt atoms is accelerated, further leading to a high activity and anti-poisoning performance of the resulting Pt_(3)Bi_(3)Zn catalyst. This work provides new insights and robust strategy for highly efficient MOR electrocatalyst with extraordinary anti-poisoning performance and stability.

关键词： fuel cells Ternary nanoplates Durability Methanol oxidation reaction Anti-poisoning

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Electrochemical disproportionation strategy to in-situ fill cation vacancies with Ru single atoms

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Nano research 2022年第6期15卷 4980-4985页

作者： Kang Xiao Run-Tong Lin Jin-Xin Wei Nan Li Hui Li Tianyi Ma Zhao-Qing Liu School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials/Guangzhou key laboratory for Clean Energy and Materials Guangzhou UniversityGuangzhou 510006China Centre for Translational Atomaterials Swinburne University of TechnologyHawthornVIC 3122Australia School of Science RMIT UniversityMelbourneVIC 3000Australia

supported single-atom catalysts(SACs)possess high catalytic activity,selectivity,and atom ***,the atom coordination environments of SACs are difficult to accurately regulate due to the high complexity of coordination site and local environment of ***,we develop an in-situ electrochemical cation-exchange method to fill the cation vacancies in MnO_(2)with Ru single atoms(SAs).This obtained catalyst exhibits high mass activity,which is~44 times higher than commercial RuO2 catalyst and excellent stability,superior to the most state-of-the-art oxygen evolution reaction(OER)*** experimental and theoretical results confirm that the doped Ru can induce charge density redistribution,resulting in the optimized binding of oxygen species,and the strong covalent interaction between Ru and MnO2 for resisting oxidation and *** work will provide a new concept in the synthesis of well-defined local environments of supported SAs.

关键词： single-atom catalysts MnO_(2) Ru disproportionation oxygen evolution reaction

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Controllably partial removal of thiolate ligands from unsupported Au_(25) nanoclusters by rapid thermal treatments for electrochemical CO_(2)reduction

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Journal of Energy Chemistry 2023年第11期86卷 16-22,I0002页

作者： Liting Huang Yongfeng Lun Yuping Liu Liming Chen Bowen Li Shuqin Song Yi Wang The key Lab of Low-carbon Chemistry&Energy Conservation of guangdong province PCFM LabSchool of Chemical Engineering and TechnologySchool of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275GuangdongChina

Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ***,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported[Au_(25)(PET)_(18)]-nanoclusters with the preservation of the core *** procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment,avoiding the reconfiguration or agglomeration of Au_(25)nanoclusters,where the degree of dethiolation can be regulated by the control of *** work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution ***,the activity and selectivity towards CO formation in electrochemical CO_(2)reduction reaction of Au_(25)nanoclusters can be *** work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.

关键词： Gold nanoclusters Thiolates Ligand removal Electrochemically active surface area Electrochemical CO_(2)reduction

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