Journal of Materials Chemistry A最新文献

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Synergistic structural and functional design of thiolated ZIF nanosheets for accelerated and selective uranium extraction 用于加速和选择性铀提取的硫化ZIF纳米片的协同结构和功能设计
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta05398j
Wen Yao,Siyuan Yu,Juanjuan Yang,Shuangyi Zhu,Tianxin Li,Hongwen Liu,Jie Yang,Xinrong Guo
{"title":"Synergistic structural and functional design of thiolated ZIF nanosheets for accelerated and selective uranium extraction","authors":"Wen Yao,Siyuan Yu,Juanjuan Yang,Shuangyi Zhu,Tianxin Li,Hongwen Liu,Jie Yang,Xinrong Guo","doi":"10.1039/d6ta05398j","DOIUrl":"https://doi.org/10.1039/d6ta05398j","url":null,"abstract":"Efficient and selective uranium extraction from seawater is a significant challenge in energy utilization. Conventional materials often exhibit poor performance due to limited mass transfer and a lack of specific recognition sites. Here, a rational design strategy with synergistic structural and functional features was proposed, and a thiolated material (ZIF-A-SH5) with a hierarchical nanosheet structure was successfully prepared for uranium capture. Its unique self-assembled nanosheet structure provided superior mass transfer channels, effectively overcoming the diffusion bottlenecks associated with traditional ZIFs. Additionally, the grafted –SH groups offered high-affinity sites for uranium. The results demonstrated that ZIF-A-SH5 achieved a theoretical maximum adsorption capacity of up to 94.42 mg g−1, ultra-fast reaction kinetics, excellent adsorption selectivity in complex ionic matrices, and stable recyclability. X-ray photoelectron spectroscopy and density functional theory calculations revealed that its superior performance resulted from a unique coordination mechanism: strong S–U coordination interactions formed between thiol groups and uranyl ions. Furthermore, the material's remarkable selectivity against competing ions was quantitatively rationalized by a significant thermodynamic preference (ΔE = 0.53 eV) for uranium, confirming a highly covalent and selective S/N synergistic coordination pathway. This work presents a promising adsorbent for practical uranium extraction from seawater and provides important theoretical guidance for designing advanced functional materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067407","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Magnetic proximity-induced spin injection suppresses singlet oxygen for durable water electrolysis 磁邻近诱导自旋注入抑制单线态氧用于持久水电解
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta04728a
Lin Wu,Yuhang Lei,Lixiang Li,Han Zhang,Lin Tao,Hongwei Zhao,Qingdong Li,Xueyuan Zhang,Chengguo Sun,Dongying Ju,Baigang An
{"title":"Magnetic proximity-induced spin injection suppresses singlet oxygen for durable water electrolysis","authors":"Lin Wu,Yuhang Lei,Lixiang Li,Han Zhang,Lin Tao,Hongwei Zhao,Qingdong Li,Xueyuan Zhang,Chengguo Sun,Dongying Ju,Baigang An","doi":"10.1039/d6ta04728a","DOIUrl":"https://doi.org/10.1039/d6ta04728a","url":null,"abstract":"While spin polarization accelerates the oxygen evolution reaction (OER) kinetics, the parasitic generation of singlet oxygen (1O2) triggers oxidative degradation of catalytic active sites, limiting the lifespan of water electrolysis. Herein, we design a 1D directionally ordered CoFeB/CoFe-LDH (CFB/LDH) heterostructure to realize spin-injection via the magnetic proximity effect (MPE). Through exchange coupling, the ferromagnetic CFB core breaks the local spin symmetry of the ultrathin LDH shell. Under a magnetic field (MF), this MPE-induced spin alignment dynamically steers the OER toward the lattice oxygen mechanism. By enforcing spin conservation, the parallel-aligned heterostructure promotes effective interfacial spin filtering, which suppresses the 1O2 pathway by 6% h−1 in favor of ground-state triplet oxygen. Consequently, the MPE-driven catalyst achieves a 36 mV reduction in OER overpotential. When integrated into a practical anion-exchange membrane water electrolyzer, it delivers a cell voltage of 1.78 V at 500 mA cm−2, representing a 40 mV reduction compared to the cell without MF, and sustains stable operation for 200 h with a negligible potential increase. This work establishes MPE-induced spin injection as a materials-design strategy for coupling interfacial spin polarization with durable and efficient water electrolysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"11 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interfacial ion–electron coupling enables synergistic solar evaporation, hydrovoltaic electricity generation, and photocatalytic degradation 界面离子-电子耦合使协同太阳能蒸发、水力发电和光催化降解成为可能
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta06132j
Chunhui Shi,Xiaoming Cao,Peng Kong,Fengqin Tang,Yunxiang Xiao,Ke Tian,Shiyu Jia,Beibei Sun,Weiliang Tian,Libing Hu
{"title":"Interfacial ion–electron coupling enables synergistic solar evaporation, hydrovoltaic electricity generation, and photocatalytic degradation","authors":"Chunhui Shi,Xiaoming Cao,Peng Kong,Fengqin Tang,Yunxiang Xiao,Ke Tian,Shiyu Jia,Beibei Sun,Weiliang Tian,Libing Hu","doi":"10.1039/d6ta06132j","DOIUrl":"https://doi.org/10.1039/d6ta06132j","url":null,"abstract":"Solar-driven systems capable of simultaneously producing freshwater, removing pollutants, and generating energy offer a promising solution to interconnected water-energy-environment challenges. However, the interplay between ion transport and electron transfer in multifunctional platforms remains poorly understood, hindering the rational design of integrated systems. Herein, we developed a vermiculite (VM)-supported CNTs/MoS2 heterostructured membrane (VM/CNTs@MoS2), which demonstrated that interfacial ion–electron coupling governed its solar evaporation, photocatalytic, and hydrovoltaic behaviors. X-ray photoelectron spectroscopy and density functional theory calculations revealed spontaneous charge redistribution at the CNTs/MoS2 heterointerface, leading to the formation of a built-in electric field (BIEF) that promoted charge separation and electron transport. Coupled with directional ion migration through negatively charged VM nanochannels, this electronically coupled structure established an efficient ion–electron transport pathway. As a result, the VM/CNTs@MoS2 membrane achieved a solar evaporation rate of 2.44 kg m−2 h−1 with an energy conversion efficiency of 92.62% and simultaneously generated a stable hydrovoltaic output with an open-circuit voltage of 0.40 V and a maximum power density of 370 mW m−2 under one-sun illumination, while retaining excellent salt tolerance and operational stability. Moreover, the enhanced interfacial charge utilization enabled MoS2 to generate hydroxyl radicals favorable for 91.2% degradation of methylene blue within 8 h. Mechanistic investigations revealed that evaporation-induced ionic flux and interfacial electron transport are dynamically coupled through the engineered heterointerface. The dynamic coupling between these ionic and electronic processes served as the common origin of the enhanced evaporation, photocatalytic activity, and electricity generation. This work establishes interfacial ion–electron coupling as an effective strategy for integrating water purification, environmental remediation, and energy generation within a single platform, providing new insights into the design of next-generation solar-driven multifunctional systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"57 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Insights into the MoS Lithium-Ion Battery Lithiation Mechanism via Big Data Electrochemical Analysis 基于大数据电化学分析的MoS锂离子电池锂化机理研究
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta03464k
Alexandar Dimitrov Marinov,Ami R. Shah,Christopher A Howard,Patrick Cullen
{"title":"Insights into the MoS Lithium-Ion Battery Lithiation Mechanism via Big Data Electrochemical Analysis","authors":"Alexandar Dimitrov Marinov,Ami R. Shah,Christopher A Howard,Patrick Cullen","doi":"10.1039/d6ta03464k","DOIUrl":"https://doi.org/10.1039/d6ta03464k","url":null,"abstract":"Molybdenum disulfide (MoS2) is a potential alternative to the commercial graphite anode in lithium-ion batteries (LIBs) due to its higher theoretical capacity (670 mAh/g) and natural earth abundance. However, the deep discharge potential range (3.00 – 0.01 V) enabling MoS2 high specific capacities is highly debated and suffers from a rapid degradation process (< 40 cycles). To investigate the MoS2 deep lithiation mechanism, long-term electrochemical testing, restrictive potential ranges after an initial deep discharge, and in situ electrochemical impedance spectroscopy (EIS) were applied. Electrochemical analysis reveals that the three cathodic reactions (labelled G, H, and I) are either parallel or series-independent, forming reversible redox couples with the single anodic peak (W). The inclusion of each additional cathodic peak increases cell capacity but accelerates capacity decay. As the redox peaks responsible for the high initial capacities vanish, we verify that capacity is stored entirely through capacitance in the long term (> 40 cycles). Our electrochemical analysis highlights that current MoS2 lithiation mechanism proposals are unable to accurately describe the phenomena observed when restricting the potential range of MoS2 after deep lithiation. Therefore, we propose a set of three electrochemical conditions that must be justified by any lithiation mechanism hypothesis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"5 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Remote Ir Single Atoms Boost RuO2 Nanoclusters for Durable Acidic Oxygen Evolution Catalysis 远程Ir单原子增强RuO2纳米团簇用于持久的酸性析氧催化
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta07383b
Xinye Zhang,Mengtian Huo,Xiaowen Gu,Xing-Zhe Guo,Ming Yang,Zihao Xing,Chi Cao,Meiling Xiao,Jinfa Chang
{"title":"Remote Ir Single Atoms Boost RuO2 Nanoclusters for Durable Acidic Oxygen Evolution Catalysis","authors":"Xinye Zhang,Mengtian Huo,Xiaowen Gu,Xing-Zhe Guo,Ming Yang,Zihao Xing,Chi Cao,Meiling Xiao,Jinfa Chang","doi":"10.1039/d6ta07383b","DOIUrl":"https://doi.org/10.1039/d6ta07383b","url":null,"abstract":"RuO2 offers a cost-effective alternative to IrO2 for acidic OER, yet its practical application is severely constrained by instability arising from lattice oxygen participation. Herein, we construct a hybrid catalyst (RuO2@Irsac-NC) in which RuO2 nanoclusters and atomically dispersed Ir single sites are co-anchored on nitrogen-doped carbon with spatial separation. This configuration enables remote electronic modulation of RuO2 via the conductive carbon support, effectively suppressing Ru over-oxidation and redirecting the OER pathway from the lattice oxygen mechanism to the adsorbate evolution route, as evidenced by in situ DEMS and Raman spectroscopy. The catalyst delivers an ultralow overpotential of 153 mV at 10 mA cm -2 and sustains stable operation over 200 h. In a two-electrode electrolyzer, it achieves overall water splitting at 1.47 V with durability exceeding 145 h. Theoretical calculations reveal that the remote interaction downshifts the Ru d-band center, lowers the *O→*OOH energy barrier, and accelerates *OH desorption. This work establishes a remote-synergy paradigm for designing durable, high-performance acidic OER catalysts with practical viability for industrial electrolysis for green hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"36 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Plasmonic truncated bipyramidal BiVO–CuSe heterostructures for efficient dual-channel HO photosynthesis 高效双通道HO光合作用的等离子体截断双锥体BiVO-CuSe异质结构
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta05362a
Qijun Xu,Chenchen Meng,Meng Zhang,Wenhao Zhang,Jiahui Zhang,Shaokai Du,Yang Zhang,Xiaohong Li,Louzhen Fan,Yunchao Li
{"title":"Plasmonic truncated bipyramidal BiVO–CuSe heterostructures for efficient dual-channel HO photosynthesis","authors":"Qijun Xu,Chenchen Meng,Meng Zhang,Wenhao Zhang,Jiahui Zhang,Shaokai Du,Yang Zhang,Xiaohong Li,Louzhen Fan,Yunchao Li","doi":"10.1039/d6ta05362a","DOIUrl":"https://doi.org/10.1039/d6ta05362a","url":null,"abstract":"Photocatalytic H2O2 synthesis has attracted significant interest for its green and low-cost nature, yet its practical application is severely limited by low yields caused by sluggish kinetics, high thermodynamic barriers, and poor light harvesting. Herein, we report the rational design of BiVO4–Cu2−xSe (BVO–CS) S-scheme heterostructures via selective photodeposition of plasmonic Cu2−xSe onto the (010) facets of truncated bipyramidal BiVO4 microcrystals. This multifunctional architecture concurrently orchestrates staggered band-edge alignment, spatially separated redox centers, and near-infrared (NIR) localized surface plasmon resonance (LSPR) activity, enabling broadband solar harvesting, unidirectional charge flow, and spatially decoupled redox half-reactions. Impressively, under vis-NIR irradiation in pure water, the optimized BVO–CS-3 catalyst achieves an exceptional H2O2 yield of 17.15 mmol g−1 h−1 within 60 min, with the cumulative H2O2 concentration reaching 7.77 mM after 240 min. Comprehensive investigations reveal a synergistic dual-channel pathway: the two-electron oxygen reduction reaction (ORR) preferentially proceeds on the conduction band of Cu2−xSe, while the two-electron water oxidation reaction (WOR) occurs on the valence band of BiVO4, with NIR-excited LSPR hot electrons substantially lowering the ORR activation barrier. Proof-of-concept experiments demonstrate that in situ generated H2O2 efficiently degrades four organic dyes simultaneously, underscoring its strong oxidative potential. This study establishes a paradigm for advanced photocatalyst design through the strategic synergy of band structure engineering, interfacial regulation, and plasmonic enhancement, offering a robust platform for efficient solar-to-chemical energy conversion.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"40 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bimetallic CeCu-MOF for selectively electroreduction of CO2 to CH4 双金属CeCu-MOF选择性电还原CO2为CH4
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta07041h
Fang-Fang Wang,Shao-Xia Wang,Peng Wang,Wei-Yin Sun
{"title":"Bimetallic CeCu-MOF for selectively electroreduction of CO2 to CH4","authors":"Fang-Fang Wang,Shao-Xia Wang,Peng Wang,Wei-Yin Sun","doi":"10.1039/d6ta07041h","DOIUrl":"https://doi.org/10.1039/d6ta07041h","url":null,"abstract":"Developing efficient electrocatalysts for CO2 reduction to high-valued hydrocarbons remains a significant challenge. Herein, we report a bimetallic MOF catalyst, CeCu-HHTP (H6HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene), that combines bimetallic synergistic effects with a two-dimensional (2D) conductive MOF architecture, for selective CO2-to-CH4 conversion. Incorporation of Cu active sites into the Ce-HHTP framework establishes strong electronic coupling between Ce and Cu, effectively tuning the electronic structure of Cu and optimizing the adsorption of key intermediates of *COOH, *CO, *CHO, *OCH3 along the CO2 reduction pathway. The optimized CeCu-HHTP-10 exhibits enlarged electrochemical active surface area, enhanced CO2 adsorption and accelerated interfacial charge-transfer kinetics. As a result, CeCu-HHTP-10 achieves a CH4 Faradaic efficiency (FE) of 70.1% and a CH4 partial current density of -144.0 mA cm-2 at -1.3 V vs. RHE, maintaining superior stability over 25 h of continuous electrolysis. In-situ ATR-SEIRAS studies and density functional theory (DFT) calculations reveal that the CeCu bimetallic MOF promotes the formation of *COOH and *CHO intermediates and lowers the energy barriers for hydrogenation, guiding the reaction pathway toward CH4 formation. This work provides a strategy for designing rare earth-transition metal bimetallic conductive MOFs and offers insights for enhancing activity and selectivity in CO2 electroreduction to valuable fuels.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Horizontal Alignment of Ti3 C2 Tx MXene Nanosheets via Spray Coating Ti3 C2 Tx MXene纳米片的水平定向喷涂
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta07110d
Nilupuli C Rathnayaka,Luke C Henderson,Žan Simon,Piers Coia,Ashleigh L Farnsworth,Kilahney Murphy,Peter Lynch,Bhagya Dharmasiri
{"title":"Horizontal Alignment of Ti3 C2 Tx MXene Nanosheets via Spray Coating","authors":"Nilupuli C Rathnayaka,Luke C Henderson,Žan Simon,Piers Coia,Ashleigh L Farnsworth,Kilahney Murphy,Peter Lynch,Bhagya Dharmasiri","doi":"10.1039/d6ta07110d","DOIUrl":"https://doi.org/10.1039/d6ta07110d","url":null,"abstract":"Controlling the orientation of two-dimensional (2D) nanomaterials is important for translating their intrinsic nanoscale properties into high-performance macroscopic systems. Among these materials, Ti 3 C 2 T x MXene has attracted significant attention due to its excellent electrical conductivity, mechanical properties, and processability, where controlled nanosheet alignment can substantially improve functional performance. However, existing MXene alignment methods are generally limited to flat substrates and lack scalability for complex geometries.Here, a scalable spray-coating strategy is demonstrated for producing horizontally aligned MXene-based UV-curable composite coatings on both flat and complex topological surfaces.MXene-polymer inks, containing varying MXene loadings (0.375-3 wt%), were formulated and spray coated through sequential thin-layer deposition followed by rapid UV curing. WAXS analysis confirmed significant in-plane alignment of MXene nanosheets, achieving Herman's orientation factors up to 0.83, comparable to conventional alignment methods such as blade coating. Rheological investigations of the MXene ink revealed that shear-thinning behavior during spraying promotes nanosheet alignment, while rapid thixotropic recovery stabilizes the aligned structure before curing. In addition, spray coating enabled aligned and patterned coatings on substrates with complex geometries and surface structures. This work establishes spray coating as a scalable platform capability for producing alignment-controlled MXene surface coatings and provides a broader framework for extending shear-induced alignment strategies to other anisotropic nanomaterial-polymer systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067401","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Continuous Solar-Driven CO2 Reduction to Liquid Oxygenates in a Scalable Photoelectrochemical Flow Cell 在可扩展的光电化学液流电池中,连续太阳能驱动的二氧化碳还原成液态氧
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta06334a
Lakshman S Sundar Arumugam,Cristopher Tinajero,Luis David Lisintuña,Ana Gutiérrez-Blanco,Javier Esteban Durantini,Victor Sans,Sixto Gimenez
{"title":"Continuous Solar-Driven CO2 Reduction to Liquid Oxygenates in a Scalable Photoelectrochemical Flow Cell","authors":"Lakshman S Sundar Arumugam,Cristopher Tinajero,Luis David Lisintuña,Ana Gutiérrez-Blanco,Javier Esteban Durantini,Victor Sans,Sixto Gimenez","doi":"10.1039/d6ta06334a","DOIUrl":"https://doi.org/10.1039/d6ta06334a","url":null,"abstract":"The transition toward low-carbon chemical manufacturing requires scalable strategies to convert carbon emissions into value-added commodities independently of fossil feedstocks. Solar-driven photoelectrochemical (PEC) CO2 conversion represents a promising pathway, yet performance is frequently bottlenecked by poor mass transport and restricted device scalability.Herein, we report a versatile, modular, 3D-printed PEC flow reactor designed for continuous and scalable CO2 utilization. The system integrates a structurally engineered BiVO4/CoP photoanode for water oxidation with a highly selective Cu-coated gas diffusion electrode (Cu/GDL) cathode, operating at an active area of 1.6 cm 2 (substantially outscaling conventional millimeter-scale laboratory cells). Coupled with online micro-GC, benchtop NMR, and in-situ Raman spectroscopy, the integrated platform enables real-time product monitoring and molecular-level tracking of potential-dependent surface intermediates *COtop and *CObridge.Under optimized continuous-flow conditions, the reactor delivers a remarkable photocurrent density of 4.5 mA•cm -2 at 1.75 V, yielding an overall cathodic Faradaic Efficiency (FE) of 95%. Remarkably, the system channels selectivity predominantly toward high-value liquid oxygenates, achieving maximum FEs of 51.6% for acetate and 41.7% for methanol. Backed by over 100 hours of continuous operational stability with robust structural preservation of the electrodes, this work provides a scalable, technologically viable blueprint for efficient solar-tochemical conversion.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
TiS-derived multiphase catalytic interfaces unlock fast hydrogen desorption in the MgH–Si hydrogen storage system ti衍生的多相催化界面解锁了MgH-Si储氢系统中的快速氢解吸
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-09-28 DOI: 10.1039/d6ta05030a
Xin Ji,Zhinian Li,Li Wang,Wei Chen,Zhengming Gao
{"title":"TiS-derived multiphase catalytic interfaces unlock fast hydrogen desorption in the MgH–Si hydrogen storage system","authors":"Xin Ji,Zhinian Li,Li Wang,Wei Chen,Zhengming Gao","doi":"10.1039/d6ta05030a","DOIUrl":"https://doi.org/10.1039/d6ta05030a","url":null,"abstract":"Among various strategies for improving the thermodynamic properties of MgH2, the MgH2–Si hydrogen storage system has attracted considerable attention due to its ability to reconstruct the dehydrogenation pathway. The introduction of Si effectively reduces the reaction enthalpy to 36.4 kJ mol−1 H2, enabling theoretical hydrogen desorption under ambient conditions. Despite these favorable thermodynamic characteristics, hydrogen desorption is still severely limited by sluggish kinetics. In this study, TiS2 was introduced into the MgH2–Si system via high-energy ball milling to optimize dehydrogenation kinetics. As a result, the onset desorption temperature of MgH2–Si–TiS2 is significantly reduced to 140.0 °C, which is 92.2 °C lower than that of the ball-milled MgH2–Si. At 250 °C, the composite can release approximately 4.00 wt% H2 within only 10 min, whereas only 3.90 wt% H2 was released for pristine MgH2–Si for 150 min. The dehydrogenation activation energy of MgH2–Si–TiS2 was 89.28 kJ mol−1, indicating markedly enhanced dehydrogenation kinetics. Experimental characterization reveals that the in situ generated MgS, TiH2 and Ti5Si3 construct a multiphase synergistic catalytic system, providing abundant heterogeneous phase interfaces for the nucleation of Mg2Si. TiH2 works as a hydrogen pump, while MgS weakens the Mg–H bonds and, together with Ti5Si3, increases the interfacial density. Their synergistic effect greatly accelerates the dehydrogenation process. The DFT calculations further reveal that TiS2, in cooperation with Si, modulates the electronic environment at the interface and enhances electron transfer. The superior catalytic mechanism of TiS2 offers a clear and facile strategy for various composite hydrogen storage systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067404","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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