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Advanced 3D ordered electrodes for PEMFC applications: From structural features and fabrication methods to the controllable design of catalyst layers

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Green energy & Environment 2024年第9期9卷 1336-1365页

作者： Kaili Wang Tingting Zhou Zhen Cao Zhimin Yuan Hongyan He Maohong Fan Zaiyong Jiang School of Chemistry & chemical engineering and Environmental engineering Weifang University Beijing key laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences College engineering and Physical Sciences and School of Energy Resources University of Wyoming

The catalyst layers(CLs) electrode is the key component of the membrane electrode assembly(MEA) in proton exchange membrane fuel cells(PEMFCs). Conventional electrodes for PEMFCs are composed of carbon-supported, ionomer, and Pt nanoparticles, all immersed together and sprayed with a micron-level thickness of CLs. They have a performance trade-off where increasing the Pt loading leads to higher performance of abundant triple-phase boundary areas but increases the electrode cost. Major challenges must be overcome before realizing its wide commercialization. Literature research revealed that it is impossible to achieve performance and durability targets with only high-performance catalysts, so the controllable design of CLs architecture in MEAs for PEMFCs must now be the top priority to meet industry goals. From this perspective, a 3D ordered electrode circumvents this issue with a support-free architecture and ultrathin thickness while reducing noble metal Pt loadings. Herein, we discuss the motivation in-depth and summarize the necessary CLs structural features for designing ultralow Pt loading electrodes. Critical issues that remain in progress for 3D ordered CLs must be studied and characterized. Furthermore, approaches for 3D ordered CLs architecture electrode development, involving material design, structure optimization, preparation technology, and characterization techniques, are summarized and are expected to be next-generation CLs for PEMFCs. Finally, the review concludes with perspectives on possible research directions of CL architecture to address the significant challenges in the future.

关键词： PEMFC 3D ordered electrode Structural features Preparation technology Ultralow Pt loading

Thermogravimetric characteristics of corn straw and bituminous coal copyrolysis based the ilmenite oxygen carriers

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Chinese Journal of chemical engineering 2024年第4期68卷 8-15页

作者： Pengxing Yuan Xiude Hu Jingjing Ma Tuo Guo Qingjie Guo College of chemical engineering Qingdao University of Science&TechnologyQingdao 266042China State key laboratory of High-efficiency Utilization of Coal and Green chemical engineering Ningxia UniversityYinchuan 750021China

Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass *** results reveal that the participation of OCs weakens the devolatilization intensity of *** the CS blending ratio isenergy in the range of 26.35-40.57 kJ·mol^(-1).

关键词： Oxygen carrier Co-pyrolysis Biomass Coal

Electrochemical reconstruction: a new perspective on Sn metal-organic complex microbelts as robust anode for lithium storage

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Rare Metals 2024年第1期43卷 76-86页

作者： Jin-Ke Shen Nai-Teng Wu Li-Yuan Wang Gang Jiang Dong-Lei Guo Jin Li Gui-Long Liu Hong-Yu Mi Huan Pang Xian-Ming Liu key laboratory of Function-oriented Porous Materials of Henan Province College of Chemistry and Chemical EngineeringLuoyang Normal UniversityLuoyang 471934China State key laboratory of Chemistry and Utilization of Carbon Based energy resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830046China School of Chemistry and chemical engineering Institute for Innovative Materials and EnergyYangzhou UniversityYangzhou 225009JiangsuChina

Tin-based materials with high theoretical capacity and suitable working voltage are ideal anode materials for lithium-ion batteries(LIBs). However, to overcome their shortcomings(volume expansion and inferior stability), the preparation processes are usually complicated and expensive. Herein, a tin-based metal-organic complex(tin 1,2-benzenedicarboxylic acid, Sn-BDC)with one-dimensional microbelt morphology is synthesized by a facile, rapid and low-cost co-precipitation method, and served as anode material for LIBs without any post-treatment. Sn-BDC exhibits a high reversible capacity with609/440 m Ah·g^(-1) at 50/2000 m A·g^(-1), and robust cycling stability of 856 m Ah·g^(-1) after 200 cycles at 200 m A·g^(-1),which are obviously superior to that of the Sn Ox/C counterparts. Moreover, an electrochemical reconstruction perspective on the lithium storage mechanism of Sn-BDC is proposed by systematic ex-situ characterizations. The reconstructed SnO_(2) replaces Sn-BDC and becomes the active material in the subsequent cycles. As the by-product of the lithiation reaction, the formed Li-based metal-organic complex(Li-BDC, wrapped around the reconstructed SnO_(2)) plays an important role in alleviating volume expansion and accelerating the charge transfer *** work is beneficial to design and construct the new electrode materials based on the electrochemical reconstruction for advanced LIBs.

关键词： Electrochemical reconstruction Metal-organic complex Anode Lithium storage mechanism Lithium-ion batteries

Subnanometric bimetallic Pt-Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu Li Tao Cai Yanran Feng Xia Liu Ning Wang Qiming Sun Institute of Sustainable energy and resources College of Chemistry and Chemical EngineeringKey Laboratory of Shandong Provincial Universities for Functional Molecules and MaterialsQingdao UniversityQingdao 266071China Innovation Center for chemical Sciences College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China

The solvolysis of ammonia borane(AB)and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical *** strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic *** this work,subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1(S-1)zeolites through a ligand-protected in-situ hydrothermal synthesis *** synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt_(0.5)Pd_(0.5)@S-1-H catalyst,affording exceptional turnover frequency(TOF)values of 1,043 and 573 mol_(H_(2))mol_(metal)^(-1)min^(-1)for AB hydrolysis and methanolysis at ambient conditions,respectively,surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O-H cleavage of water,thereby facilitating the H_(2) production from AB ***,a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes,with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation,giving a high TOF value of 1,260 h^(-1)under atmospheric *** study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials,but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation

A zincophilic molecular brush for a dendrite-free,corrosionresistant,zinc metal anode with a long life cycle

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Nano Research 2024年第1期17卷 390-396页

作者： Penggao Liu Jia Guo Xinyue Chen Ting Wang Yanping Huang Shasha Gao Tao Wang Dongling Wu Kaiyu Liu State key laboratory of Chemistry and Utilization of Carbon based energy resources College of ChemistryXinjiang UniversityUrumqi 830017China Hunan Provincial key laboratory of chemical Power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China key laboratory of New Low-carbon Green chemical Technology School of Chemistry and Chemical EngineeringEducation Department of Guangxi Zhuang Autonomous RegionGuangxi UniversityNanning 530004China key laboratory of Microelectronics and energy of Henan Province Department of Physics and Electronic EngineeringXinyang Normal UniversityXinyang 464000China Interdisciplinary Research Center for Sustainable energy Science and engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001China

Zinc-based aqueous rechargeable batteries have attracted extensive attention due to their low cost,safety,and environmental ***,dendrite growth and hydrogen evolution of Zn anodes limit their large-scale application.A new strategy to produce a polyacrylamide/reduced graphene oxide(PAM@rGO)molecular nanobrush coating and control Zn electrolyte interface engineering is proposed for use in highly reversible Zn plating/*** evolution is inhibited,and Zn deposition is consolidated using the rich zincophilic functional groups of the branched polyacrylamide chain and the high conductivity of *** to the synergistic effects of corrosion resistance and dendrite-free growth,PAM@rGO/Zn provides prolonged and reversible Zn plating/*** functional theory(DFT)calculations expand on homogenized *** PAM@rGO/Zn||activated carbon(AC)capacitor exhibits long cyclic stability,fast ion transfer,and minimal interfacial *** study provides experimental and theoretical bases for the structural design of Zn anode.

关键词： zincophilic nanobrush polyacrylamide/reduced graphene oxide(PAM@rGO)/Zn surface modification Zn based energy storage

Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

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Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma key laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State key laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and chemical engineering Anhui UniversityHefei 230601People’s Republic of China School of chemical engineering The University of AdelaideAdelaideSA 5005Australia State key laboratory of High‑Efficiency Utilization of Coal and Green chemical engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial key laboratory of Advanced energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of chemical engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia ***,relevant out-lab research is still in its ***,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 *** to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long ***,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed *** as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic *** work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid

Facile preparation of coal-based ultramicroporous carbon microspheres for selective CO_(2)capture

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Carbon resources Conversion 2024年第3期7卷 97-105页

作者： Mei An Tuo Guo Qingjie Guo Jiangmen laboratory of Carbon Science and Technology the Hong Kong University of Science and Technology(Guangzhou)JiangmenGuangzhou 529000China State key laboratory of High-efficiency Coal Utilization and Green chemical engineering School of Chemistry and Chemical EngineeringNingxia UniversityYinchuanNingxia 750021China key laboratory of Clean chemical engineering in Universities of Shandong College of Chemical EngineeringQingdao University of Science&TechnologyQingdao 266042China

The basic structure of aromatic compounds that are abundant in coal is the carbonaceous precursor derived from carbon ***,it remains to be a huge challenge to prepare carbon microspheres using coal due to the complex construction and composition of ***,a simple and viable way to obtain coal-based microporous carbon microspheres was developed by means of ethanol pyrolysis and a sequential extraction *** as-prepared carbon microsphere featured aspherical micron particles of a uniform size(0.6-1.6㎛),abundant O-functional groups,excellent thermal stability,high SBET(415.5-983.2 m^(2)/g),and plentiful ultra-micropores(63.15-72.72%).The coal-based carbon microsphere exhibited a noteworthy CO_(2)uptake(3.19-4.97 mmol/g at 273 K and 1.0 bar),acceptable CO_(2)/N_(2)selectivity(IAST:23-46)and moderate isosteric heats(20-32 kJ/mol).This synthetic strategy is important for the preparation of ultramicroporous carbon microspheres using coal,and the synthetic carbon microspheres have promising prospects for highly efficient CO_(2)capture.

关键词： Coal Ultramicroporous Carbon microspheres Ethanolysis Sequential extraction CO_(2)capture

Electronic modulation of sprout-shaped NiCoP nanoarrays by N and Ce doping for efficient overall water splitting

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Nano Research 2024年第1期17卷 282-289页

作者： Ting Zhao Guancheng Xu Bingbing Gong Jiahui Jiang Li Zhang State key laboratory of Chemistry and Utilization of Carbon Based energy resources College of ChemistryXinjiang UniversityUrumqi 830017China College of chemical engineering Xinjiang UniversityUrumqi 830017China

Bifunctional catalysts for hydrogen/oxygen evolution reactions(HER/OER)are urgently needed given the bright future of water splitting hydrogen production ***,the self-supporting N and Ce dual-doped NiCoP nanoarrays(denoted N,Ce-NiCoP/NF)grown on Ni foam are successfully *** the N,Ce-NiCoP/NF simultaneously acts as the HER and OER electrodes,the voltages of 1.54 and 2.14 V are obtained for driving 10 and 500 mA·cm^(-2)with a robust durability,and demonstrate its significant potential for practical water *** to both experiments and calculations,the electronic structure of NiCoP may be significantly altered by strategically incorporating N and Ce into the lattice,which in turn optimizes the Gibbs free energy of HER/OER intermediates and speeds up the water splitting ***,the sprout-shaped morphology significantly increases the exposure of active sites and facilitates charge/mass transfer,thereby augmenting catalyst *** study offers a potentially effective approach involving the regulation of anion and cation double doping,as well as architectural engineering,for the purpose of designing and optimizing innovative electrocatalysts.

关键词： transition metal phosphides overall water splitting elements doping nanoarrays

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