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Strategies to achieve effective nitrogen activation

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Carbon Energy 2024年第5期6卷 137-163页

作者： Bin Chang Huabin zhang Shuhui Sun gaixia zhang KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)ThuwalKingdom of Saudi Arabia Institut National de la Recherche Scientifique(INRS) CentreÉnergie Matériaux TélécommunicationsVarennesQuébecCanada Department of Electrical Engineering École de Technologie Supérieure(ÉTS)MontréalQuébecCanada

Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.

关键词： activation via mediators catalyst optimization electrochemical nitrogen fixation high-energy activation of nitrogen nitrogen

Advancements on metal oxide semiconductor photocatalysts in photo-electrochemical conversion of carbon dioxide into fuels and other useful products

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Frontiers in Energy 2024年第2期18卷 187-205页

作者： Jai PRAKASH zhangsen CHEN Shakshi SAINI gaixia zhang Shuhui SUN Department of Chemistry National Institute of Technology HamirpurHamirpur 177005India Institut National de la Recherche Scientifique(INRS) Centre Énergie Matériaux TélécommunicationsVarennes J3X 1P7Canada Department of Chemistry Indian Institute of Technology MandiHimachal PradeshIndia Department of Electrical Engineering École de Technologie SupérieureMontréal H3C 1K3Canada

Due to its fascinating and tunable optoelectronic properties,semiconductor nanomaterials are the best choices for multidisciplinary applications.Particularly,the use of semiconductor photocatalysts is one of the promising ways to harness solar energy for useful applications in the field of energy and environment.In recent years,metal oxide-based tailored semiconductor photocatalysts have extensively been used for photocatalytic conversion of carbon dioxide(CO_(2))into fuels and other useful products utilizing solar energy.This is very significant not only from renewable energy consumption but also from reducing global warming point of view.Such current research activities are promising for a better future of society.The present mini-review is focused on recent developments(2–3 years)in metal oxide semiconductor hybrid photocatalysts-based photo-electrochemical conversion of CO_(2)into fuels and other useful products.First,general mechanism of photo-electrochemical conversion of CO_(2)into fuels or other useful products has been discussed.Then,various metal oxide-based emerging hybrid photocatalysts including tailoring of their morphological,compositional,and optoelectronic properties have been discussed with emphasis on their role in enhancing photoelectrochemical efficienty.Afterwards,mechanism of their photo-electrochemical reactions and applications in CO_(2)conversion into fuels/other useful products have been discussed.Finally,challenges and future prospects have been discussed followed by a summary.

关键词： metal-oxide semiconductors nanohybrid photocatalysts photo-electrochemical CO_(2)conversion tailoring morphology fuels challenges and future prospects

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

Atomically Dispersed Transition Metal-Nitrogen-Carbon Bifunctional Oxygen Electrocatalysts for Zinc-Air Batteries:Recent Advances and Future Perspectives

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Nano-Micro Letters 2022年第2期14卷 257-281页

作者： Fang Dong Mingjie Wu zhangsen Chen Xianhu Liu gaixia zhang Jinli Qiao Shuhui Sun Institut National de La Recherche Scientifique(INRS)-CentreÉnergie Matériaux Télécommunications VarennesQC J3X 1P7Canada Key Laboratory of Materials Processing and Mold Ministry of EducationZhengzhou UniversityZhengzhou 450002People’s Republic of China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringShanghai Innovation Institute for MaterialsDonghua UniversityShanghai 201620People’s Republic of China Engineering Research Center of Nano Geomaterials of Ministry of EducationChina University of GeosciencesWuhan 430074People’s Republic of China

Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.

关键词： Atomically dispersed metal-nitrogen-carbon Oxygen evolution reaction(OER) Oxygen reduction reaction(ORR) Bifunctional oxygen electrocatalysts Zinc-air batteries(ZABs)

Energetics and thermodynamic stability of potential Fe (II) -hexa-aza-active sites for O_(2) reduction in PEM fuel cells

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SusMat 2022年第6期2卷 731-748页

作者： Vassili P.Glibin Jean-Pol Dodelet gaixia zhang Department of Chemical and Biochemical Engineering University of Western OntarioLondon OntarioCanada Institut National de la Recherche Scientifique(INRS) Energie Materiaux Telecommunications Research CentreVarennesQuebecCanada Department of Electrical Engineering Ecole de Technologie Superieure(ETS)1100rue Notre-Dame OuestMontrealQuebec H3C 1K3Canada

We present here a thermodynamic assessment of the stability behavior in acid environment at 298 and 353 K(80◦C)of two iron(II)hexa-aza-macrocyclic complexes and of an hexa-aza-iron-based site(Fe^(II)N_((4+2))/C)that should potentially be active for the oxygen reduction reaction in proton exchange membrane(PEM)fuel cells.The calculations of the equilibrium constant(K c)for the demetallation reaction indicate that the iron(II)-hexa-aza-macrocyclic complexes and Fe^(II)N_((4+2))/C are chemically stable in an acid medium at 298 and 353 K.Compared with two other potential model sites(Fe^(II)N_((4+2))/C and Fe II N(2+2)/C)that were thought to be present in the same Fe-based catalysts,K c of Fe^(II)N_((4+2))/C is two to three orders of magnitude smaller at 353 K,and three to four orders of magnitude smaller at 298 K,than K c for Fe^(II)N_((4+2))/C or Fe II N(2+2)/C,revealing the great chemical stability of Fe^(II)N_((4+2))/C.In this work,we discuss about a novel proposition that the two catalytic sites active in these Fe-based catalysts are Fe II N_(4)/C and Fe^(II)N_((4+2))/C.This proposition is in agreement with the durability behavior of these catalysts in PEM fuel cells and also with their known physico-chemical characterizations.The origin of the fast and slow decay behaviors of the different sites,which are active at the Fe–N–C-based cathode of PEM fuel cells,is also discussed.

关键词： active site fuel cell oxygen reduction reaction thermodynamic stability

Atomically Dispersed Fe-Co Bimetallic Catalysts for the Promoted Electroreduction of Carbon Dioxide

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Nano-Micro Letters 2022年第2期14卷 79-93页

作者： zhangsen Chen gaixia zhang Yuren Wen Ning Chen Weifeng Chen Tom Regier James Dynes Yi Zheng Shuhui Sun Institut National de la Recherche Scientifique-Énergie Matériaux et Télécommunications VarennesQC J3X 1P7Canada School of Materials Science and Engineering University of Science and Technology100083 BeijingPeople’s Republic of China Canadian Light Source University of SaskatchewanSaskatoonSK S7N 2V3Canada Research Institute of Photocatalysis State Key Laboratory of Photocatalysis on Energy and EnvironmentFuzhou UniversityFuzhou 350116People’s Republic of China

The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.

关键词： CO_(2)reduction Electrocatalysis Syngas production Cobalt Iron Bimetallic catalysts

3D Grid of Carbon Tubes with Mn3O4-NPs/CNTs Filled in their Inner Cavity as Ultrahigh-Rate and Stable Lithium Anode

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Energy & Environmental Materials 2023年第4期6卷 187-194页

作者： Shiping zhang Fangming Han Qijun Pan Dou Lin Xiaoguang Zhu Cheng Shao gaixia zhang Zhaoming Wang Shuhui Sun Guowen Meng Key Laboratory of Materials Physics and Anhui Key Laboratory of Nanomaterials and NanotechnologyInstitute of Solid State PhysicsHFIPSChinese Academy of SciencesP.O.Box 1129Hefei 230031China Department of Materials Science and Engineering University of Science and Technology of ChinaHefei 230026China Department of Electrical Engineering Ecole de Technologie Superieure(ETS)MontrealQuebec H3C 1K3Canada Institut National de la Recherche Scientifique(INRS) Centre EnergieMateriaux TelecommunicationsVarennesQuebec J3X 1P7Canada

Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.

关键词： 3D interconnected carbon tube arrays anode free-standing Mn_(3)O_(4)

Advanced semiconductor catalyst designs for the photocatalytic reduction of CO_(2)

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Materials Reports(Energy) 2023年第2期3卷 27-42,I0002页

作者： zhangsen Chen gaixia zhang Siyi Cao Guozhu Chen Cuncheng Li Ricardo IzquierdoShuhui Sun Institut National de la Recherche Scientifique–Centre Energie Materiaux Telecommunications VarennesQuebecJ3X 1P7Canada Department of Electrical Engineering Ecolede Technologie Superieure(ETS)MontrealQuebecH3C 1K3Canada School of Chemistry and Chemical Engineering University of JinanJinan250022PR China

Using clean solar energy to reduce CO_(2)into value-added products not only consumes the over-emitted CO_(2)that causes environmental problems,but also generates fuel chemicals to alleviate energy crises.The photocatalytic CO_(2)reduction reaction(PCO_(2)RR)relies on the semiconductor photocatalysts that suffer from high recombination rate of the photo-generated carriers,low light harvesting capability,and low stability.This review explores the recent discoveries on the novel semiconductors for PCO_(2)RR,focusing on the rational catalyst design strategies(such as surface engineering,band engineering,hierarchical structure construction,single-atom catalysts,and biohybrid catalysts)that promote the catalytic performance of semiconductor catalysts on PCO_(2)RR.The advanced characterization techniques that contribute to understanding the intrinsic properties of the photocatalysts are also discussed.Lastly,the perspectives on future challenges and possible solutions for PCO_(2)RR are presented.

关键词： Photoreduction of CO_(2) Semiconductor catalysts Photocatalyst modification Heterojunction construction Catalytic efficiency Activity Environmental and sustainable applications

Proton Exchange Membrane(PEM)Fuel Cells with Platinum Group Metal(PGM)-Free Cathode

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Automotive Innovation 2021年第2期4卷 131-143页

作者： Lei Du gaixia zhang Shuhui Sun Institut National de la Recherche Scientifique(INRS)-Énergie Matériaux et Télécommunications VarennesQC J3X 1S2Canada School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001China

Proton exchange membrane(PEM)fuel cells have gained increasing interest from academia and industry,due to its remarkable advantages including high efficiency,high energy density,high power density,and fast refueling,also because of the urgent demand for clean and renewable energy.One of the biggest challenges for PEM fuel cell technology is the high cost,attributed to the use of precious platinum group metals(PGM),e.g.,Pt,particularly at cathodes where sluggish oxygen reduction reaction takes place.Two primary ways have been paved to address this cost challenge:one named low-loading PGM-based catalysts and another one is non-precious metal-based or PGM-free catalysts.Particularly for the PGM-free catalysts,tremendous efforts have been made to improve the performance and durability-milestones have been achieved in the corresponding PEM fuel cells.Even though the current status is still far from meeting the expectations.More efforts are thus required to further research and develop the desired PGM-free catalysts for cathodes in PEM fuel cells.Herein,this paper discusses the most recent progress of PGM-free catalysts and their applications in the practical membrane electrolyte assembly and PEM fuel cells.The most promising directions for future research and development are pointed out in terms of enhancing the intrinsic activity,reducing the degradation,as well as the study at the level of fuel cell stacks.

关键词： PEM fuel cells Cathode PGM-free catalysts Performance Stability