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Direct seawater splitting for hydrogen production:Recent advances in materials synthesis and technological innovation

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Green Energy & Environment 2025年第1期10卷 11-33页

作者： Yilin Zhao Zhipeng Yu Aimin Ge Lujia Liu Joaquim Luis Faria Guiyin Xu Meifang Zhu State Key Laboratory for Modification of chemical Fibers and Polymer Materials Center for Advanced Low-dimension MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai201620China International Iberian Nanotechnology Laboratory(INL) Avenida Mestre Jose VeigaBraga4715-330Portugal The MacDiarmid Institute for Advanced Materials and Nanotechnology School of Chemical and Physical SciencesVictoria University of WellingtonWellington6012New Zealand LSRE-LCM-Laboratory of Separation and Reaction engineering-Laboratory of Catalysis and Materials Faculty of EngineeringUniversity of PortoRua Dr.Roberto Frias s/nPorto4200-465Portugal ALiCE-Associate Laboratory in chemical engineering Faculty of EngineeringUniversity of PortoRua Dr.Roberto Frias s/nPorto4200-465Portugal

Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil ***,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in ***,producing hydrogen on an industrial scale is challenging due to the high production *** present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater *** the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater *** the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater ***,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.

关键词： Seawater splitting Catalyst Membranes Mixed seawater systems Self-powered systems

Target-oriented confinement of Ru-Co nanoparticles inside N-doped carbon spheres via a benzoic acid guided process for high-efficient low-temperature ammonia synthesis

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Journal of Energy Chemistry 2021年第6期30卷 140-146,I0005页

作者： Jun Ni Zhenni Tan Qianjin Sai Jie Zhu Xiuyun Wang Bingyu Lin Jianxin Lin Chak-tong Au Lilong Jiang national engineering research center of chemical fertilizer Catalyst Fuzhou UniversityFuzhou 350002FujianChina

Ru-based heterogeneous catalysts have been used in a wide range of important ***,due to the sintering of Ru nanoparticles their practical applications are somewhat ***,for the first time we report a new and facile strategy to confine Ru and/or Co nanoparticles(NPs) in the channels of N-doped carbon using benzoic acid to guide the deposition location of *** developed catalyst with confined RuCo alloy particles exhibits high resistance against Ru sintering and displays excellent activity and long term stability for NH3 synthesis,achieving an NH3 synthesis rate of up to 18.9 mmol NH_(3) gcat^(-1)h^(-1)at 400℃,which is ca.2.25 times that of the catalyst prepared without confinement(with metal deposited on the support surface).In the latter case,there is an increase of nanoparticle size from 2.52 to 4.25 nm together with ca.48% decrease of NH_(3) synthesis rate after 68 h at 400℃.This study provides a new avenue for simple fabrication of precious-metal-based catalysts that are highly resistant against sintering,specifically suitable for low-temperature synthesis of ammonia with outstanding efficiency.

关键词： Ru-and Co-based catalysts Ammonia synthesis Confinement Sintering resistance Nanoparticle size

Efficient catalytic removal of COS and H_(2)S over graphitized 2D micro-meso-macroporous carbons endowed with ample nitrogen sites synthesized via mechanochemical carbonization

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Green Energy & Environment 2022年第5期7卷 983-995页

作者： Xun Kan Guanqing Zhang Yingying Luo Fujian Liu Yong Zheng Yihong Xiao Yanning Cao Chak-tong Au Shijing Liang Lilong Jiang national engineering research center of chemical fertilizer Catalyst(NERC-CFC) School of Chemical EngineeringFuzhou UniversityFuzhou350002China

Developing a suitable catalyst for the elimination of highly toxic carbonyl sulfide(COS)and hydrogen sulfide(H_(2)S) is of great significance in terms of industrial safety and environmental *** demonstrate here the facile synthesis of graphitized 2D micro-meso-macroporous carbons by one-step carbonization of a mixture of urea and glucose at 700–900℃.The as-synthesized graphitized catalysts,designated as 2DNHPC-x(x=urea/glucose mass ratio),are endowed with an ultra-high concentration(12.9–20.2 wt%)of stable and versatile nitrogen sites(*** and pyridine)which are anchored on the surface via stable covalent *** a result,the 2D-NHPC-x are active in catalytic hydrolysis of COS on pyrrolic N to H_(2)S,and the H_(2)S can be subsequently captured on pyridinic N and converted to elemental sulfur at ambient conditions over the same *** the prepared catalysts,2D-NHPC-x can catalytically hydrolysize 91%of COS to H_(2)S at 30℃,whereas the conversion ratio over the common catalysts g-C_(3)N_(4)and Fe_(2)O_(3)are below 6.0%.Furthermore,these catalysts also exhibit H_(2)S conversion and sulfur selectivity of nearly 100%at 180℃with long-time durability,which is higher than those of the most reported carbonbased *** contrast,the H_(2)S capacities of activated carbon,ordered mesoporous carbons(OMC)and N-doped OMC are 3.9,1.5 and2.39 mmol g^(-1),*** the experimental and theoretical results are disclosed that 2D-NHPC-x are superior to the nitrogen-doped porous materials ever applied in simultaneous catalytic elimination of both COS and H_(2)S.

关键词： carbons catalytic endowed

Pyrochlore La_(2)Zr_(2-x)Ni_(x)O_(7)anodes for direct ammonia solid oxide fuel cells

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Frontiers in Energy 2024年第5期18卷 699-711页

作者： Shiqing Yang Yijie Gao Xinmin Wang Fulan Zhong Huihuang Fang Yu Luo Lilong Jiang national engineering research center of chemical fertilizer Catalyst(NERC-CFC) College of Chemical EngineeringFuzhou UniversityFuzhou 350002China

Developing efficient anode catalysts for direct ammonia solid oxide fuel cells(NH_(3)-SOFCs)under intermediate-temperatures is of great importance,in support of hydrogen economy via ammonia *** the present work,the pyrochlore-type La_(2)Zr_(2-x)Ni_(x)O_(7+δ)(LZN_(x),x=0,0.02,0.05,0.08,0.10)oxides were synthesized as potential anode catalysts of NH_(3)-SOFCs due to the abundant Frankel defect that contributes to the good conductivity and oxygen ion mobility *** effects of different content of Ni^(2+)doping on the crystal structure,surface morphology,thermal matching with YSZ(Yttria-stabilized zirconia),conductivity,and electrochemical performance of pyrochlore oxides were examined using different characterization *** findings indicate that the LZN_(x)oxide behaves as an n-type semiconductor and exhibits an excellent high-temperature chemical compatibility and thermal matching with the YSZ ***,LZN_(0.05)exhibits the smallest conductive band potential and bandgap,making it have a higher power density as anode material for NH_(3)-SOFCs compared to other *** a result,the maximum power density of the LZN_(0.05)-40YSZ composite anode reaches 100.86 mW/cm^(2)at 800℃,which is 1.8 times greater than that of NiO-based NH_(3)-SOFCs(56.75 mW/cm^(2))under identical flow rate and temperature *** extended durability indicates that the NH_(3)-SOFCs utilizing the LZN_(0.05)-40YSZ composite anode exhibits a negligible voltage degradation following uninterrupted operation at 800℃for 100 h.

关键词： anode catalyst ammonia oxidation Ni particles NH_(3)-SOFCs

Synergistically S/N self-doped biochar as a green bifunctional cathode catalyst in electrochemical degradation of organic pollutant

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Green Energy & Environment 2025年第1期10卷 214-230页

作者： Xuechun Wang Huizhong Wu Jiana Jing Ge Song Xuyang Zhang Minghua Zhou Raf Dewil Key Laboratory of Pollution Process and Environmental Criteria Ministry of EducationCollege of Environmental Science and EngineeringNankai UniversityTianjin300350China Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution Nankai UniversityTianjin300350China Tianjin Advanced Water Treatment Technology International Joint research center College of Environmental Science and EngineeringNankai UniversityTianjin300350China Department of chemical engineering KU LeuvenJ.De Nayerlaan 5Sint-Katelijne-Waver B2860Belgium

Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable ***,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)*** the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 *** functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) *** pyridinic N and thiophene S were the main active sites responsible for_OH generation,N vacancies were the active sites to produce ^(1)O_(2) from *** performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 *** is also industrially applicable,achieving satisfactory performance treating in real water *** system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.

关键词： Biochar S and N self-doping H_(2)O_(2)production In-situ FTIR Metal-free electrochemical advanced oxidation processes

Enhancing the activity of MoS_(2)/SiO_(2)-Al_(2)O_(3) bifunctional catalysts for suspended-bed hydrocracking of heavy oils by doping with Zr atoms

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Chinese Journal of chemical engineering 2021年第11期34卷 126-134页

作者： Yongde Ma Rengan Liang Wenquan Wu Jiayin Zhang Yanning Cao Kuan Huang Lilong Jiang national engineering research center of chemical fertilizer Catalyst(NERC-CFC) Fuzhou UniversityFuzhou 350002China

Developing catalysts with not only hydrogenation activity but also cracking activity is very important for the advancement of suspended-bed hydrocracking *** this respect,MoS_(2)/SiO_(2)-Al_(2)O_(3)bifunctional catalyst is a kind of typical catalysts with both hydrogenation and cracking ***,a series of Zr-doped SiO_(2)-Al_(2)O_(3)mixed oxides were synthesized by a sol-gel coupled with hydrothermal *** synthesized mixed oxides were characterized for chemical structures and acidic *** is found that doping SiO_(2)-Al_(2)O_(3)with Zr atoms significantly increases the numbers of acidic *** Zr-doped SiO_(2)-Al_(2)O_(3)mixed oxides were then combined with dispersed MoS_(2),which was in-situ produced from oil-soluble Mo precursors,to fabricate a novel kind of bifunctional catalysts for suspended-bed hydrocracking of heavy *** to the significantly increased numbers of acidic sites in Zr-doped SiO_(2)-Al_(2)O_(3)mixed oxides,corresponding bifunctional catalysts demonstrate much enhanced activity for suspended-bed hydrocracking of heavy oils in relative to MoS_(2)/SiO_(2)-Al_(2)O_(3)bifunctional catalysts.

关键词： Petroleum Hydrogenation Catalyst Suspended bed Cracking Mixed oxide

Preparation and Characterization of Carbon Nanotubes-Coated Cordierite for Catalyst Supports

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Journal of Natural Gas Chemistry 2006年第3期15卷 211-216页

作者： Jianmei Wang Rong Wang Xiujin Yu Jianxin Lin Feng Xie Kemei Wei national engineering research center of chemical fertilizer Catalyst Fuzhou University Fuzhou 350002 China

The carbon nanotubes-coated cordierite （CNTs-cordierite） was fabricated by pyrolysis of ethine on cordierite with iron catalyst, which was penetrated into the cordierite substrate by vacuum impregnation. The cordierite substrate, carbon naontubes, and CNTs-cordierite were characterized by SEM, TEM/HREM, BET, and TGA. The results show that the carbon nanotubes were distributed uniformly on the surface of cordierite. A significant increase in BET surface area and pore volume was observed, and a suitable pore-size distribution was obtained. On the CNTs-cordierite, carbon nanotubes penetrated into the cordierite substrate, which led to a remarkable stability of the CNTs against ultrasound maltreatment. Growth time is an important factor for thermostability and texture of the sample. The mass increased but the purity decreased with the growth time, which caused the exothermic peak shift to low temperature, and the corresponding full width half maximum （FWHM） of the peak in DTG increased.

关键词： carbon nanotube cordierite pyrolysis ethine catalyst support

Deciphering Water Oxidation catalysts:The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu Chun‑Hua Yan State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key Laboratory of Baiyunobo Rare Earth Resource researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing national Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis

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Chinese chemical Letters 2023年第1期34卷 461-464页

作者： Chuanfeng Zhang Siyu Shi Biyun Fang Jun Ni Jianxin Lin Xiuyun Wang Bingyu Lin Lilong Jiang national engineering research center of chemical fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350002China

The development of effective Ru catalyst for ammonia synthesis is of important practical value and scientific significance because of the wide application of ammonia as a fertilizer and its promising applications in the renewable ***,ZrO_(2) was regarded as an inferior support for Ru catalyst used in ammonia *** we prepare ZrO_(2) with monoclinic phase and carbon species from ZrCl_(4) following the preparation route of UiO-66 as well as ammonia *** to the presence of a larger amount of hydrogen adsorption as well as the easier desorption of hydrogen species,the ill effect of hydrogen species on the nitrogen adsorption-desorption and ammonia synthesis can be effectively *** resulting ZrO_(2)-supported Ru catalyst showed 4 times higher ammonia synthesis activity than the conventional Ru/ZrO_(2) obtained from zirconium nitrate.

关键词： Ru catalyst ZrO_(2) Carbon Hydrogen adsorption-desorption Ammonia synthesis