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Porous organic material-based atomically dispersed metal electrocatalysts

ENERGY & ENVIRONMENTAL SCIENCE 2025年第9期18卷 3986-4009页

作者： Zhang, Hao wang, suwen Lv, Enmin Qi, Menghui He, Chengchao Dong, Xinglong Qiu, Jieshan wang, Yong Wen, Zhenhai MIT Dept Chem Engn Cambridge MA 02139 USA Univ Oxford Dept Chem Oxford OX1 3TA England Zhejiang Univ Inst Catalysis Dept Chem Adv Mat & Catalysis Grp Hangzhou 310058 Peoples R China Dalian Univ Technol Sch Mat Sci & Engn Dalian 116024 Peoples R China Chinese Acad Sci Fujian Inst Res Struct Matter CAS Key Lab Design & Assembly Funct Nanostruct Fuzhou 350002 Fujian Peoples R China Chinese Acad Sci Fujian Inst Res Struct Matter Fujian Prov Key Lab Mat & Tech Hydrogen Energy Fuzhou 350002 Fujian Peoples R China Beijing Univ Chem Technol Coll Chem Engn Beijing 100029 Peoples R China

The transition to renewable energy sources and the need for efficient energy conversion technologies have led to the development of various types of catalysts, among which atomically dispersed metal catalysts (ADMCs) supported by porous organic materials (POMs) have attracted attention for their high catalytic efficiency and stability. This review focuses on the development and application of ADMCs supported by POMs, such as MOFs, COFs, and HOFs, which offer catalytic performance due to their high atomic utilization, stability, and selectivity. This paper systematically explores various strategies for synthesizing ADMCs, including the use of organic linkers, metal nodes, and pore spaces within POMs to stabilize metal atoms and prevent aggregation. Key applications highlighted include energy conversion and storage technologies, such as fuel cells, water splitting, CO2 reduction and nitrogen reduction, where ADMCs demonstrate the potential to replace noble metals. Despite the progress, challenges remain in achieving high metal loading, long-term stability, and cost-effective large-scale production. This study underscores the importance of advanced characterization techniques and computational models to deepen the understanding of ADMCs' catalytic mechanisms and guide future material design, paving the way for their broader application in sustainable energy technologies.

关键词： Energy efficiency

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Bifunctional Built-In Electric Field Across the Interface of Single Molecule and 2D Matrix Supramolecular Assembly for Highly Efficient and Selective Photocatalytic CO2 Reduction

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ADVANCED FUNCTIONAL MATERIALS 2025年第0期

作者： Xu, Cui Zhang, Mengyang Gao, Qiang Li, Teng wang, suwen wang, Yun Liu, Yunpeng Peng, Hui-Qing Zhang, Wenjun Liu, Bin Beijing Univ Chem Technol Coll Chem Beijing Adv Innovat Ctr Soft Matter Sci & Engn State Key Lab Chem Resource Engn Beijing 100029 Peoples R China Griffith Univ Sch Environm & Sci Ctr Catalysis & Clean Energy Gold Coast Qld 4222 Australia Chinese Acad Sci Inst High Energy Phys Beijing 100049 Peoples R China City Univ Hong Kong Ctr Superdiamond & Adv Films COSDAF Kowloon Tat Chee Ave Hong Kong Peoples R China City Univ Hong Kong Dept Mat Sci & Engn Kowloon Tat Chee Ave Hong Kong Peoples R China

The sluggish interfacial charge transfer and constrained intrinsic catalytic activity in photocatalytic systems are major obstacles to the efficiency and selectivity of CO2 photoreduction (CO2PR). Herein, a novel organic-inorganic supramolecular assembly heterojunction (NiAl-ZnTCPP) comprising single molecules and 2D matrix is presented, featuring high-quality interfacial contact achieved through electrostatic interactions and hydrogen bonding. This comprehensive investigations unveil the formation of an effective interfacial built-in electric field (BEF) directed from NiAl-LDH toward ZnTCPP, which significantly boosts the activity and selectivity of CO2PR. NiAl-ZnTCPP achieves an impressive CO yield of 1568.6 mu mol g(-1) h(-1), exceeding the yields of ZnTCPP and NiAl-LDH by 25 and 5.6 times, respectively, while maintaining a remarkable 98% CO selectivity and extremely low hydrogen selectivity. Utilizing advanced experimental technologies, including diverse operando characterizations and theoretical simulations, the bifunctionality of the BEF is elucidated, which not only accelerates the transfer of photogenerated carriers from photosensitizer to NiAl-ZnTCPP, but also enhances the intrinsic activity of NiAl-ZnTCPP by modulating the electronic structure of nickel active sites (specifically lowering the energy barrier for *COOH to *CO conversion while improving charge transport capability). This work provides new insights into the application of molecule/2D matrix junctions to generate interfacial electric fields that enhance photocatalytic performance.

关键词： bifunctional built-in electric field charge transfer CO2 photoreduction intrinsic catalytic activity single molecule/2D matrix assembly

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Synergistic Engineering of Electron-Enriched Nickel Sites for Highly Efficient Photocatalytic CO2 Reduction to C2H6

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ADVANCED FUNCTIONAL MATERIALS 2025年第6期35卷

作者： Xu, Cui Yu, Sha Zhang, Mengyang Zhan, Xinyue Jiang, Shuai wang, suwen Liu, Guihao Ren, Jing Sun, Xiaoliang wang, Yun Peng, Hui-Qing Liu, Bin Zhang, Wenjun Song, Yu-Fei Beijing Univ Chem Technol State Key Lab Chem Resource Engn Beijing Adv Innovat Ctr Soft Matter Sci & Engn Coll Chem Beijing 100029 Peoples R China Griffith Univ Ctr Catalysis & Clean Energy Sch Environm & Sci Gold Coast Qld 4222 Australia City Univ Hong Kong Ctr Super Diamond & Adv Films COSDAF Kowloon Tat Chee Ave Hong Kong Peoples R China City Univ Hong Kong Dept Mat Sci & Engn Kowloon Tat Chee Ave Hong Kong Peoples R China

The production of multi-carbon compounds through CO2 photoreduction (CO2PR) holds great promise but faces challenges due to high kinetic barriers and the sluggish process of C-C coupling. Overcoming these obstacles requires fine engineering of active sites. In this study, Ni active sites are engineered through the synergistic effect of metal-oxo cluster (Mo7O246-) and hydroxyl vacancy (V-OH). In contrast to the Ni sites unmodified with Mo7O246- and V-OH, which are unable to produce multi-carbon products, the constructed electron-enriched Ni active sites exhibit an impressive selectivity of up to 43.02% and a high yield rate of 246.70 mu mol g(-1) h(-1) for C2H6, which represent one of the best results for CO2PR to C2H6. Through a comprehensive investigation involving operando experiments and theoretical simulations, hydroxyl vacancy and the formed Mo & horbar;O & horbar;Ni bonds is demonstrated due to the filling of hydroxyl vacancies with oxygen atoms from Mo7O246- synergistically constructed electron-rich Ni sites. Such Ni sites efficiently catalyze CO2 conversion to C2H6 by enhancing the adsorption of *CO, promoting subsequent hydrogenation, and enabling low energy barriers for CO2 hydrogenation to *OCOH and the coupling of *CH3 intermediates. This study provides deeper insights into the photocatalytic process, highlighting the significance of tailored active sites for efficient CO2 conversion.

关键词： active site engineering CO2 photoreduction mechanism study multi-carbon product vacancy and intercalation

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The Dual Role of Urban Vegetation: Trade-Offs Between Thermal Regulation and Biogenic Volatile Organic Compound Emissions

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ATMOSPHERE 2025年第4期16卷 385-385页

作者： Dong, Wen Ma, Danping Lin, Song Ye, Shen wang, suwen Shen, Li Chen, Dan Qiu, Yingying Yang, Bo Cheng, Tianliang Zhang, Jing Chen, Jian Ren, Yuan Zhejiang A&F Univ Sch Forestry & Biotechnol 666 Wusu St Hangzhou 311300 Zhejiang Peoples R China Zhejiang Univ Water Resources & Elect Power Sch Hydraul Engn Hangzhou 310018 Peoples R China Zhejiang Prov Publ Welf Forests & State Owned Fore Hangzhou 311300 Peoples R China Tianmushan Forest Ecosyst Orientat Observat & Res Hangzhou 311300 Peoples R China

Under the dual pressures of global warming and accelerated urbanization, urban green spaces (UGS) serve as crucial yet paradoxical elements, alleviating urban heat island (UHI) effects while emitting biogenic volatile organic compounds (BVOCs) that exacerbate air pollution;however, their spatial trade-offs remain underexplored. This study bridges this gap by developing an Urban Heat Mitigation Index (HMI) and a BVOC flux accounting framework integrating remote sensing and field observations. The results showed that (1) the cooling effect exhibits significant spatial heterogeneity, with continuous green networks around West Lake and along the Qiantang River forming efficient cooling corridors (HMI > 0.75), while fragmented green spaces in northeastern areas show weaker cooling effects (HMI < 0.35);(2) BVOC emission intensity displays a "high suburbs-low centers" pattern, with suburban areas emitting 1.9-2.3 times more BVOCs than urban centers, while BVOC-induced PM2.5 (0.02-0.05 mu g m(-3)) and O-3 (12-33 mu g m(-3)) concentrations in city centers still pose significant health risks;(3) spatial analysis reveals a weak positive correlation between HMI and BVOC emissions (Moran's I = 0.096, p < 0.05), with four distinct coupling patterns identified: "high cooling-low emissions" (17.5% of area), "low cooling-high emissions" (1.1%), "high cooling-high emissions" (18.7%), and "low cooling-low emissions" (3.9%). This study provides quantitative evidence for optimizing UGS layouts to balance ecological benefits and environmental risks, emphasizing the importance of vegetation screening and spatial allocation in sustainable urban planning.

关键词： heat island effect green space sustainable development ecosystem services trade-offs

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Two-dimensional materials for NOx reduction to ammonia: From electrocatalyst to system

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COORDINATION CHEMISTRY REVIEWS 2025年 535卷

作者： wang, suwen Xia, Junkai Yang, Xiaohui Xie, Qian Zhuang, Zechao Feng, Huajun Xiang, Hai Chen, Zuliang Li, Hui Zhang, Lei Li, Yongfu Yu, Bing Ma, Tianyi Zhejiang A&F Univ State Key Lab Subtrop Silviculture Hangzhou 311300 Peoples R China Zhejiang A&F Univ Ecol Environm & Hlth Coll EEHC Hangzhou 311300 Peoples R China Tsinghua Univ Dept Chem Beijing 100084 Peoples R China Fujian Normal Univ Sch Environm & Resource Sci Fujian Key Lab Pollut Control & Resource Reuse Fuzhou 350007 Fujian Peoples R China RMIT Univ Ctr Atomaterials & Nanomfg CAN Sch Sci Melbourne Vic 3000 Australia ARC Ind Transformat Res Hub Intelligent Energy Eff Melbourne Vic 3000 Australia

Ammonia is a globally produced commodity chemical that is essential in supporting the needs of an expanding population. The traditional Haber-Bosch process for the production of ammonia, although effective, encounters obstacles stemming from its reliance on fossil fuels and substantial energy expenditure. The electrocatalytic NOx reduction reaction (NOxRR) for ammonia synthesis has recently captured interest as a compelling alternative due to its high efficiency and environmentally friendly characteristics. Two-dimensional (2D) materials, with their numerous exposed active sites, substantial specific surface area, excellent conductivity, and readily adjustable electronic properties, offer significant potential for activating NOx species in sustainable NOxRR applications. This review highlights the latest research advancements in the use of 2D materials for electrochemical NOx reduction. We began by providing an overview of the fundamental principles of electrochemical NOx reduction. Next, we introduced recent progress in this field using 2D materials such as graphene, MXene, metal alloys/ sulfides, layered double hydroxides, and carbon nitride. We then summarized the state-of-the-art electrochemical systems employed in NOxRR processes. Finally, we discussed the challenges and prospects of NOxRR based on 2D materials, aiming for large-scale industrial implementation in the near future.

关键词： Two-dimensional materials NO x reduction Ammonia synthesis Electrochemical systems Fundamental principles

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Magnetic-Field-Induced Spin Transition in Single-Atom Catalysts for Nitrate Electrolysis to Ammonia

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Nano Letters 2025年第21期25卷 2025 May 13页

作者： You, Xingchao Guo, Zhongyuan Jiang, Qiuling Xia, Junkai wang, suwen Yang, Xiaohui Zhuang, Zechao Li, Yongfu Xiang, Hai Li, Hao Yu, Bing National Key Laboratory for Development and Utilization of Forest Food Resources Zhejiang A&F University Hangzhou 311300 China Ecological-Environment & Health College (EEHC) Zhejiang A&F University Hangzhou 311300 China Advanced Institute for Materials Research (WPI-AIMR) Tohoku University Sendai 980-8577 Japan College of Environmental and Resource Sciences Zhejiang University Hangzhou 310058 China Department of Chemistry Tsinghua University Beijing 100084 China

Electrochemical nitrate reduction (NitRR) using single-atom catalysts (SACs) offers a promising pathway for sustainable ammonia production. Herein, we explore the use of external magnetic fields to regulate the spin state of Ru SACs supported on nitrogen-doped carbon (Ru-N-C), aiming to optimize their catalytic performance toward NitRR. Under magnetic field conditions, Ru-N-C exhibits a remarkable NH₃ yield rate of ∼38 mg L^-1 h^-1 and a Faradaic efficiency of ∼95% over 200 h. Our spectroscopic and magnetic characterization demonstrates that the external magnetic field induces a spin transition to a high-spin state in Ru SACs/N-C. Theoretical analysis further suggests that the increased spin state of Ru shifts the density of states away from the Fermi level, weakening the adsorption affinity for *NH₂. Economic analysis hints at cost effectiveness and scalability. Overall, this study demonstrates that magnetic-field-induced spin modulation effectively optimizes NitRR electrocatalysts. © 2025 The Authors. Published by American Chemical Society.

关键词： ammonia synthesis magnetic field nitrate reduction reaction single-atom catalysis spin-state transition

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Synthesis and characteristics of proton-conducting membranes based on cerium sulfophenyl phosphate and poly (2, 5-benzimidazole) by hot-pressing method

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 2011年第17期36卷 11068-11074页

作者： Dong, Feilong Li, Zhongfang wang, suwen wang, Zhenhai Shandong Univ Technol Sch Chem Engn Zibo 255049 Shandong Peoples R China

Cerium sulfophenyl phosphate (CeSPP), a novel proton conductor, is prepared starting from mixtures of m-sulfophenyl phosphonic acid (msPPA) and ammonium ceric nitrate. The CeSPP samples are combined with poly (2, 5-benzimidazole) (ABPBI) to prepare ABPBI/CeSPP composite membranes by polyphosphoric acid (PPA) hot-pressed method. The ABPBI/CeSPP composite membranes are characterized by X-ray diffraction (XRD) and infrared spectroscopy (IR). Thermogravimetric analysis (TGA) indicates thermal stability of the composite membranes below 200 degrees C. Scanning electron microscopy (SEM) indicates that CeSPP particles are homogenously dispersed into the composite membranes. Ce, P and S atoms are well illustrated and uniformly distributed in composite membranes via energy-dispersive X-ray spectroscopy (EDX) analysis. The proton conductivity of membrane doped in 38 wt.% CeSPP reaches 0.14 Scm(-1) at 180 degrees C under 100% relative humidity. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

关键词： Composite membranes Poly (2, 5-benzimidazole) Cerium sulfophenyl phosphate m-sulfophenyl hosphonic acid

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Preparation and characterization of zirconium sulfophenyl phosphate-doped sulfonated poly(phthalazinone ether sulfone) composite proton exchange membrane

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IONICS 2013年第7期19卷 1027-1036页

作者： wang, suwen Jin, Lei Li, Zhongfang Shandong Univ Technol Sch Chem Engn Zibo 255049 Shandong Peoples R China

Polymer composite membranes based on sulfonated poly(phthalazinone ether sulfone) (SPPES) and zirconium sulfophenyl phosphate (ZrSPP) were prepared. Three ZrSPP concentrations were used: 10, 20, and 30 wt%. The membranes were characterized by infrared spectroscopy (IR), X-ray diffraction spectroscopy, thermal gravimetric analysis, and scanning electron microscopy (SEM). The IR results indicated the formation of intense hydrogen bonds between ZrSPP and SPPES molecules. The SEM micrographs showed that ZrSPP well dispersed with SPPES and form a lattice structure. The proton conductivity of the SPPES (degree of sulfonation (DS) 64 %)/ZrSPP (10 wt%) composite membrane reached 0.39 S/cm at 120 A degrees C 100 % relative humidity and that of the 30 wt% of SPPES (DS 16.1 %)/ZrSPP composite membrane reached 0.18 S/cm at 150 A degrees C. The methanol permeabilities of the SPPES/ZrSPP composite membranes were in the range of 2.1 x 10(-8) to 0.13 x 10(-8) cm(2)/s, much lower than that of NafionA (R) 117 (10(-6) cm(2)/s). The composite membranes exhibited good thermal stabilities, proton conductivities, and good methanol resistance properties.

关键词： Composite Proton exchange membrane Sulfonated poly(phthalazinone ether sulfone) Zirconium sulfophenyl phosphate

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Proton-conducting membrane preparation based on SiO₂-riveted phosphotungstic acid and poly (2,5-benzimidazole) via direct casting method and its durability

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JOURNAL OF MATERIALS SCIENCE 2012年第11期47卷 4743-4749页

作者： wang, suwen Dong, Feilong Li, Zhongfang Shandong Univ Technol Sch Chem Engn Zibo 255049 Shandong Peoples R China

SiO2-riveted phosphotungstic acid (T-PWA-SiO2) was synthesized using the sol-gel method and thermally treated in a microwave synthesizer. The dissolving-detaching experiment shows that PWA in T-PWA-SiO2 exhibits better fastness than in the sample without thermal treatment (PWA-SiO2). The T-PWA-SiO2 samples were then combined with poly(2,5-benzimidazole) (ABPBI) to prepare ABPBI/(T-PWA-SiO2) composite membranes using the polyphosphoric acid direct-castingmethod. These composite membranes were characterized through X-ray diffraction and infrared spectroscopy. Then, the T-PWA-SiO2 particles were combined with ABPBI through hydrogen bonding between PWA and C = N in ABPBI. Membrane morphologies were investigated using scanning electron microscopy. Results of the thermogravimetric analysis indicate thermal stability of the composite membranes below 200 degrees C. The proton conductivity and durability between ABPBI/(T-PWA-SiO2) and ABPBI/(PWA-SiO2) composite membranes were also compared. The conductivity and life of the composite membranes were enhanced using T-PWA-SiO2. The conductivity of the ABPBI/(T-PWA-SiO2) (46 wt%) composite membrane was approximately 0.055 S/cm at 180 degrees C under 100% relative humidity.

关键词： PROTON exchange membrane fuel cells PHOSPHOTUNGSTIC acids SILICA BENZIMIDAZOLES SOL-gel processes MOLDING (Chemical technology) ELECTRIC conductivity DESIGN & construction

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MnO₂ nanorod catalysts for magnesium air fuel cells: Influence of different supports

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 2015年第21期40卷 6809-6817页

作者： Yue, Panfeng Li, Zhongfang wang, suwen wang, Yuxin Shandong Univ Technol Sch Chem Engn Zibo 255049 Peoples R China Tianjin Univ Sch Chem Engn State Key Lab Chem Engn Tianjin 300072 Peoples R China

MnO2 nanorods adsorbed with different supports (non-support, carbon black, and MWCNTs) were prepared through hydrothermal method for magnesium-air fuel cells (MAFCs). The morphological characteristics of the catalysts indicate that the combination modes of nanorods and MWCNTs are parallel, cross, and bend intersect, which provide a large surface areas and enhance electron transfer process. X-ray diffraction pattern illustrates the crystal form of MnO2, and X-ray photoelectron spectroscopy reveals that the existing form of manganese is Mn4+. The ORR performance investigated using a rotating disk electrode shows that the initial reduction potential of MnO2/C and MnO2/MWCNTs in the LSV curves are -0.02 and 0.03 V vs. Hg/HgO (+0.098 V vs. NHE), respectively. The electron transfer number of MnO2/MWCNTs is 3.86, which corresponds to four electrons. In the I-t curves, the oxygen reduction current density of MnO2/MWCNTs decreases by 18.1% and MnO2/C decays by 27.9% after 60 h. The CVs reveal that the current density losses of MnO2/MWCNTs and MnO2/C are 0.4 and 0.8 mA cm(-2) after scanning for 5000 cycles. The potential values of the air electrode loaded with MnO2/C and MnO2/MWCNTs catalysts are -0.78 and -0.62 V vs. SCE, respectively, at 150 mA cm(-2), respectively. The discharge performance of a single-chamber MAFC shows that the peak power densities of MnO2/C and MnO2/MWCNTs are 60.95 and 70.47 mW cm(-2), respectively, 20 degrees C in 10 wt% NaCl solutions. The single cells of MnO2/MWCNTs can continuously discharge for more than 24 h at a current density of 20 mA cm(-2). The EIS proves that the conductivity of MnO2/MWCNTs is higher than MnO2/C. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

关键词： Magnesium-air fuel cells Oxygen reduction reaction MnO2 nanorod Supports Multi-walled carbon nanotube

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