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Boosting mechanical-to-ionic transduction for self-powered piezoionic sensing. 促进自供电压电传感的机械到离子转导。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-22 DOI: 10.1039/d5mh01784j
Juan A Guerrero, Cédric Plesse, Vladislav Y Shevtsov, Alexander S Shaplov, Jean-Marie Raquez, Jérémy Odent

In the realm of sensing, piezoionic systems have emerged as innovative tools for perceiving tactile sensations through mechanical-to-ionic transduction, mimicking biological signal production and transmission. To date, the biomimetic transduction mechanism and strategies for engineering the transduction efficiency remain not fully understood and underutilized. This review provides the fundamentals of mechanical-to-ionic transduction for efficient self-powered sensing, identifying the most crucial structural and operating parameters governing the generation of a transient signal output with respect to the migration and redistribution of ions upon mechanical stimulation. It also examines the recent strategies for efficiently converting mechanical keystrokes into electrical signals through performance-driven structural design, thereby maximizing piezoionic voltage generation. This involves engineering ion transport and fluid flow through porosity, microphase separation, conductive pathways and structural gradients. With respect to piezoionic effect-based applications, this review highlights the promising potential of polymeric, ionic materials in soft wearable electronics, ionic skins, tissue engineering, biointerfaces and energy harvesting.

在传感领域,压电系统已经成为一种创新的工具,通过机械到离子的传导来感知触觉,模仿生物信号的产生和传输。迄今为止,仿生转导机制和工程转导效率的策略仍未完全了解和充分利用。这篇综述提供了有效的自供电传感的机械到离子转导的基本原理,确定了控制在机械刺激下离子迁移和再分配的瞬态信号输出产生的最关键的结构和操作参数。它还研究了通过性能驱动的结构设计有效地将机械按键转换为电信号的最新策略,从而最大限度地提高了压电电压的产生。这涉及工程离子传输和流体通过孔隙、微相分离、导电途径和结构梯度的流动。在基于压电效应的应用方面,本文重点介绍了聚合物、离子材料在软性可穿戴电子产品、离子皮肤、组织工程、生物界面和能量收集方面的应用前景。
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引用次数: 0
Evolving electrocatalytic nitrate-to-ammonia conversion on Cu- and Co-based catalyst engineering with paired electrolysis approaches. 基于配对电解方法的铜基和钴基催化剂工程中硝酸盐到氨转化的发展。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-22 DOI: 10.1039/d5mh02001h
Nabilah Saafie, Noor Ashikin Mohamad, Wei Shan Koh, Xianhai Zeng, Soo Young Kim, Wee-Jun Ong

The electrocatalytic nitrate (NO3-) reduction reaction to ammonia (NH3) offers a sustainable pathway for wastewater remediation and distributed NH3 synthesis, presenting a capable alternative to the energy-intensive Haber-Bosch process. Copper (Cu)- and cobalt (Co)-based catalysts are among the most promising for this reaction due to their favourable electronic structure for NO3- activation and cost-effectiveness. However, their propensity for rapid deactivation caused by the strong adsorption of intermediates like *NO that poison active sites remains a primary impediment to high selectivity and stability. This review comprehensively investigates recent breakthroughs in overcoming this limitation through advanced catalyst design strategies specifically for Cu- and Co-based systems. In detail, the protocols were critically examined to regulate intermediate adsorption strength via facet engineering, oxidation state modulation, single-atom dispersion and construction of bimetallic catalysts that provide synergistic *H species to enhance hydrogenation kinetics through optimization of the d band center of Cu and Co. Furthermore, innovative tandem catalysis systems and paired electrolysis configurations are also explored to couple the NO3- reduction reaction with alternative oxidation reactions (AORs) to drastically improve energy efficiency and economic viability. Therefore, by synthesizing these design principles this review aims to guide the development of next-generation, high-performance and durable Cu- and Co-based electrocatalysts for scalable sustainable nitrogen management.

电催化硝酸(NO3-)还原反应生成氨(NH3)为废水修复和分布式NH3合成提供了可持续的途径,是能源密集型Haber-Bosch工艺的有力替代方案。铜(Cu)和钴(Co)基催化剂是最有希望用于该反应的催化剂,因为它们具有有利于NO3-活化的有利电子结构和成本效益。然而,由于*NO等中间体对活性位点的强吸附,它们的快速失活倾向仍然是高选择性和稳定性的主要障碍。这篇综述全面调查了最近在克服这一限制方面的突破,通过先进的催化剂设计策略,专门针对Cu和co基系统。详细地说,这些方案通过facet工程、氧化态调制、单原子分散和双金属催化剂的构建来调节中间吸附强度,通过优化Cu和Co的d波段中心,提供协同*H物种来增强氢化动力学。创新的串联催化系统和配对电解配置也被探索,以耦合NO3-还原反应与替代氧化反应(AORs),以大大提高能源效率和经济可行性。因此,通过综合这些设计原则,本综述旨在指导下一代高性能和耐用的Cu和co基电催化剂的开发,用于可扩展的可持续氮管理。
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引用次数: 0
A water-recyclable, robust, and self-healing sugar-based supramolecular network enabled by Maillard-analogous initialization of polymerization 一个水可循环,稳健,自我修复的糖基超分子网络,由美拉德类似的聚合初始化实现。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-22 DOI: 10.1039/D5MH01828E
Siyang Li, Tow-Jie Lok, Shi-Han Ngo, Yaoting Xue, Zhikun Miao, Tao Feng, Lei Wang, Jie-Wei Wong, Jiatee Low, Kai-Yi Lim, Min-Rou Woon, Axel T. Neffe, Tuck-Whye Wong, Tiefeng Li, Xuxu Yang and Wei Yang

Crosslinked functional polymers exhibit exceptional mechanical and chemical properties critical for applications spanning biomedical engineering, advanced adhesives, and self-healing materials. However, challenges in recycling, either due to irreversible crosslinks or, in the case of covalent adaptable networks (CANs), limited solid-state plasticity that typically requires catalysts, significantly restrict sustainability. To address these limitations, we present a novel water-mediated polymerization strategy inspired by the radical-generating mechanism of the Maillard reaction, utilizing maltose as both an initiator and a functional side group in a simple, catalyst-free, aqueous reaction with acrylamide (AAm). This mild, one-pot reaction occurs below 100 °C, forming adaptively functionalized supramolecular networks (AFSNs) that form supramolecular networks through hydrogen bonding and display dynamic imine linkages to the maltose side chains supporting self-healing and re-shaping. These elastomers are characterized by impressive mechanical strength (up to 5 MPa tensile strength), high elongation (up to 1000%), notable fracture energy (36 kJ m−2), robust adhesive performance (up to 4.8 MPa), and rapid self-healing capability at room temperature. Crucially, the elastomer's supramolecular network can be fully and repeatedly dissolved and reprocessed using only water, preserving mechanical integrity without chemical degradation. This sustainable approach provides a practical solution for synthesizing and recycling high-performance crosslinked materials while eliminating environmental hazards, guiding the future development of green polymer chemistry and functional material design.

交联功能聚合物具有卓越的机械和化学性能,对于生物医学工程、先进粘合剂和自修复材料的应用至关重要。然而,由于不可逆交联或共价适应性网络(can)有限的固态塑性(通常需要催化剂),回收方面的挑战极大地限制了可持续性。为了解决这些限制,我们在美拉德反应的自由基生成机制的启发下,提出了一种新的水介导聚合策略,利用麦芽糖作为引发剂和功能侧基,在一个简单的、无催化剂的、与丙烯酰胺(AAm)的水反应中进行。这种温和的单锅反应发生在100°C以下,形成自适应功能化的超分子网络(AFSNs),通过氢键形成超分子网络,并在麦芽糖侧链上显示动态亚胺键,支持自我修复和重塑。这些弹性体具有令人印象深刻的机械强度(抗拉强度高达5mpa)、高伸长率(高达1000%)、显著的断裂能(36kj - m-2)、强大的粘接性能(高达4.8 MPa)以及在室温下的快速自修复能力。最重要的是,弹性体的超分子网络可以完全重复溶解,并且只需要用水就可以进行再加工,从而保持机械完整性而不会发生化学降解。这种可持续的方法为高性能交联材料的合成和回收提供了一种实用的解决方案,同时消除了环境危害,指导了未来绿色高分子化学和功能材料设计的发展。
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引用次数: 0
Mechanically robust polyurethane elastomers enabled by soft-segment-regulated hydrogen bonds and microphase separation for ultrasound imaging medical catheters. 机械坚固的聚氨酯弹性体通过软段调节氢键和微相分离用于超声成像医学导管。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1039/d5mh01806d
Yanlong Luo, Qingchuang Lu, Jianye Lu, Zuqian Chen, Chichao Li, Zhenyang Luo, Wu Cai, Cheng-Hui Li, Zhengdong Fei, Qingbo Lu, Yao Liu

Conventional strategies for enhancing the mechanical robustness of thermoplastic polyurethane elastomers (TPUs) rely on hard-segment engineering, such as introducing dynamic covalent/noncovalent bonds or optimizing chain extenders, yet overlook the critical role of soft segments in governing microphase separation. Here, we present a soft-segment-regulated design that leverages crystallizable polyols to synergize hierarchical hydrogen bonding, tunable microphase separation, and strain-induced crystallization (SIC), achieving excellent mechanical performance. Among them, PU-PTMEG exhibits exceptional mechanical properties, including a tensile strength of 75.6 MPa, a toughness of 337.4 MJ m-3, and a fracture energy of 131.6 kJ mol-1-values that surpass those of many metals and alloys. Furthermore, its true fracture stress reaches 1.03 GPa, comparable to that of spider silk, while its toughness is approximately 2.3 times higher, demonstrating a remarkable combination of strength and toughness. The dynamic yet dense hydrogen bond network, strategically balanced in both strength and reversibility, enables efficient energy dissipation during deformation, while the SIC activated by aligned soft segments facilitates elastomer self-reinforcement. Finally, by combining the antibacterial properties endowed by intrinsic acylhydrazine groups (bacterial survival rate <20%) and the introduction of rigid polyurethane foam as an acoustic impedance modifier, high-contrast ultrasound imaging of TPU wires has been successfully achieved.

提高热塑性聚氨酯弹性体(tpu)机械稳健性的传统策略依赖于硬段工程,例如引入动态共价键/非共价键或优化扩链剂,但忽视了软段在控制微相分离中的关键作用。在这里,我们提出了一种软段调节设计,利用可结晶的多元醇来协同分层氢键,可调谐的微相分离和应变诱导结晶(SIC),实现了优异的机械性能。其中,PU-PTMEG具有优异的力学性能,抗拉强度为75.6 MPa,韧性为337.4 MJ - m-3,断裂能为131.6 kJ mol-1,超过了许多金属和合金。其真实断裂应力达到1.03 GPa,与蛛丝相当,而其韧性约为蛛丝的2.3倍,表现出优异的强度与韧性结合。动态而致密的氢键网络,在强度和可逆性上实现了战略平衡,可以在变形过程中有效地耗散能量,而对齐的软段激活的碳化硅有助于弹性体的自我增强。最后,结合酰基肼固有基团赋予的抗菌性能(细菌存活率)
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引用次数: 0
Approaching the Sabatier optimum via a triple-defect synergistic strategy for enhanced oxygen evolution reaction. 通过三缺陷协同策略增强析氧反应接近萨巴蒂尔最优。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1039/d5mh01997d
Danni Yang, Jingjing Wu, Tao Li, Linfeng Yi, Riyue Ge, Ziqi Sun, Hua Kun Liu, Shi Xue Dou, Ding Yuan, Yuhai Dou

The development of highly efficient and stable oxygen evolution reaction (OER) electrocatalysts represents a critical challenge for advancing water splitting hydrogen production technology. In this work, we report a novel defect engineering strategy through synergistic Fe/Al doping and Co vacancy construction in a CoMOF precursor, achieving remarkable performance enhancement after electrochemical reconstruction. Density functional theory (DFT) calculations elucidate the cooperative mechanism of Fe/Al dopants and Co vacancies, which positions the Gibbs free energy of O (ΔGO*) exactly at the center of ΔGOH* and ΔGOOH*, thereby dramatically decreasing the catalytic overpotential and boosting the catalytic activity. Experimental characterization studies conclusively demonstrate the successful electronic structure modulation achieved through this triple-defect (Fe/Al doping and Co vacancy) synergistic strategy, which exhibits exceptional electrocatalytic performance with an ultralow overpotential of 229 mV at 10 mA cm-2. The concerted effects of these engineered defects not only remarkably enhance the intrinsic activity through optimized electronic configurations but also significantly improve charge transfer kinetics. This innovative defect-engineering paradigm establishes a universal methodology for the rational design of high-performance electrocatalysts across diverse electrochemical energy conversion systems.

高效稳定的析氧反应(OER)电催化剂的开发是推进水裂解制氢技术的关键挑战。在这项工作中,我们报告了一种新的缺陷工程策略,通过在CoMOF前驱体中协同掺杂Fe/Al和Co空位构建,在电化学重建后获得了显着的性能增强。密度泛函理论(DFT)计算阐明了Fe/Al掺杂剂与Co空位的协同作用机制,使O (ΔGO*)的吉布斯自由能恰好位于ΔGOH*和ΔGOOH*的中心,从而显著降低了催化过电位,提高了催化活性。实验表征研究最终证明了通过这种三缺陷(Fe/Al掺杂和Co空位)协同策略成功实现了电子结构调制,该策略在10 mA cm-2下具有229 mV的超低过电位,具有优异的电催化性能。这些工程缺陷的协同作用不仅通过优化电子构型显著提高了本征活性,而且显著改善了电荷转移动力学。这种创新的缺陷工程范式为合理设计跨不同电化学能量转换系统的高性能电催化剂建立了一种通用的方法。
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引用次数: 0
Fullerene derivative integration controls morphological behaviour and recombination losses in non-fullerene acceptor-based organic solar cells. 富勒烯衍生物集成控制非富勒烯受体有机太阳能电池的形态行为和重组损失。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1039/d5mh02065d
Apostolos Panagiotopoulos, Kyriakos Almpanidis, Esther Y-H Hung, Nikolaos Lempesis, Weidong Xu, George Perrakis, Sandra Jenatsch, Levon Abelian, Stoichko Dimitrov, Dimitar Kutsarov, Ehsan Rezaee, Benjamin M Gallant, Vlad Stolojan, Konstantinos Petridis, Samuel D Stranks, Henry J Snaith, George Kakavelakis, S Ravi P Silva

The complex and varied relationship found in intermolecular interactions within the photo-active layers plays a decisive role in determining the photovoltaic energy conversion and overall device performance of organic solar cells (OSCs). Among different approaches, the ternary blend strategy serves as an effective technique to control the morphology within the active layer in OSCs. In this work, PM6:L8-BO is used as the main host system (binary) while the fullerene molecules PC61BM and PCBC6 are introduced to form ternary OSCs. The results highlight the important role of fullerenes in enhancing the performance of binary non-fullerene acceptor-based cells by suppressing trap-assisted recombination and optimizing the active layer morphology. The improved film phase microstructure, enabled by fullerene derivatives with higher lowest unoccupied molecular orbital (LUMO) energy levels in comparison to the host acceptor (L8-BO), facilitates more efficient charge collection and reduced non-radiative recombination. This results in an increase in the fill factor (FF) and open circuit voltage (Voc) in the ternary OSCs. Consequently, power conversion efficiencies (PCEs) of binary OSCs were increased from 17.28% to 18.10% and 18.38% for the PC61BM- and PCBC6-based ternary OSCs, respectively. Furthermore, the addition of the fullerene molecules in the active layer provided the devices with enhanced long-term photo and thermal stability. The ternary OSCs demonstrated degradation pathways distinct from those of binary cells (ISOS-L1-I and ISOS-D2-I protocols), as identified through in situ ultraviolet-visible (UV-Vis) absorption and Raman spectroscopy. Molecular dynamics (MD) simulations, for the first time, reveal the significant role of fullerene molecules as morphology regulators in non-fullerene acceptor (NFA)-based systems. Their presence ensures improved dispersion of blend components and promotes more uniform and isotropic thermal and mechanical behaviour. Finally, mini-modules with active areas of 3.8 cm2 were fabricated, achieving PCEs of 12.90%, 13.32%, and 13.70% for the binary and ternary cells using PC61BM-and PCBC6-based ternary cells, respectively. Our results demonstrate that regulation of the morphology of the photo-active layer in OSCs through fullerene incorporation reduces the non-radiative energy loss pathways, enabling high-efficiency, stable and scalable OSCs.

光活性层内分子间相互作用的复杂多变关系对有机太阳能电池的光伏能量转换和整体器件性能起着决定性作用。在不同的方法中,三元共混策略是一种有效的控制osc活性层内形貌的方法。在这项工作中,PM6:L8-BO作为主要的宿主系统(二元),并引入富勒烯分子PC61BM和PCBC6形成三元osc。研究结果强调了富勒烯通过抑制陷阱辅助重组和优化活性层形态,在提高二元非富勒烯受体细胞性能方面的重要作用。与宿主受体(L8-BO)相比,富勒烯衍生物具有更高的最低未占据分子轨道(LUMO)能级,从而改善了膜相微观结构,有利于更有效的电荷收集和减少非辐射重组。这会导致三元osc中填充因子(FF)和开路电压(Voc)的增加。因此,基于PC61BM和pcbc6的三元OSCs的功率转换效率(pce)分别从17.28%提高到18.10%和18.38%。此外,在活性层中加入富勒烯分子可以增强器件的长期光稳定性和热稳定性。通过原位紫外-可见(UV-Vis)吸收和拉曼光谱鉴定,三元osc表现出与二元细胞(iso - l1 - i和iso - d2 - i协议)不同的降解途径。分子动力学(MD)模拟首次揭示了富勒烯分子在非富勒烯受体(NFA)体系中作为形态调节剂的重要作用。它们的存在确保了混合成分的分散,促进了更均匀和各向同性的热和机械行为。最后,利用基于pc61bm和基于pcbc6的三元电池,制备出了有效面积为3.8 cm2的微型模块,分别实现了12.90%、13.32%和13.70%的pce。我们的研究结果表明,通过富勒烯掺入调节OSCs光活性层的形态可以减少非辐射能量损失途径,从而实现高效、稳定和可扩展的OSCs。
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引用次数: 0
Ordering-induced concentration effect: a mass transport boost for CO2 electroreduction. 有序诱导的浓度效应:二氧化碳电还原的质量输运提升。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1039/d5mh02031j
Zequn Han, Mengqian Li, Peipei Li, Wenya Fan, Chengbin Zhang, Haohao Duan, Zhijie Wang, Qingxia Chen, Xingchen Jiao

Electrocatalytic reduction of CO2 into CO holds great promise for addressing environmental challenges and industrial needs. However, the practical implementation is hindered by the hydrogen evolution reaction (HER), which competes for electrons and reduces the selectivity of the CO2 reduction reaction (CO2RR). Here, we have proposed a novel strategy to enhance CO2RR selectivity using an ordered structure from a mass transport perspective for the first time. Ag nanowires (NWs) were selected as model catalysts and assembled into an ordered array. The ordered structure of Ag NWs induces an ordered micro electric field that crucially regulates the kinetic mass transports of both the CO2RR and HER. This micro electric field is demonstrated to promote the preferential accumulation of CO2 on the catalyst surface while concurrently repelling H2O molecules. This dual action, which enriches the desired reactant and depletes the source for the competing reaction, tilts the balance in favor of CO2 reduction over the HER, thereby enhancing selectivity towards CO production. Therefore, the ordered Ag NW arrays demonstrated highly efficient CO2 electroreduction to CO, resulting in an impressive 97.3% faradaic efficiency (FE) of CO at a current density of 100 mA cm-2, significantly outperforming their disordered counterparts. This innovative approach not only inspires the design of structural assembly in electrocatalysts from a mass transport perspective but also provides fundamental insights into the relationship between the ordering of structured catalysts and their CO2RR performance.

电催化将CO2还原为CO对于解决环境挑战和工业需求具有很大的希望。然而,析氢反应(HER)会竞争电子,降低CO2还原反应(CO2RR)的选择性,阻碍了实际实施。本文首次从质量输运的角度提出了一种利用有序结构增强CO2RR选择性的新策略。选择银纳米线(NWs)作为模型催化剂,并将其组装成有序阵列。Ag NWs的有序结构诱导了有序的微电场,该电场对CO2RR和HER的动力学质量输运起着至关重要的调节作用。该微电场促进了CO2在催化剂表面的优先积累,同时排斥H2O分子。这种双重作用丰富了所需的反应物,同时耗尽了竞争反应的源,使平衡倾向于CO2还原而不是HER,从而提高了CO生成的选择性。因此,有序的Ag NW阵列显示出高效的CO2电还原成CO,在100 mA cm-2的电流密度下,CO的法拉第效率(FE)达到了令人印象深刻的97.3%,显著优于无序的同类。这种创新的方法不仅从质量传递的角度启发了电催化剂结构组件的设计,而且为结构催化剂的有序与其CO2RR性能之间的关系提供了基本的见解。
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引用次数: 0
Hybrid metamaterials for decoupled electromagnetic-acoustic wave manipulation: achieving four negative constitutive parameters. 去耦电磁声波操纵的杂化超材料:实现四个负本构参数。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1039/d5mh01858g
Zhaolun Yu, Tian Gan, Xiaole Wang, Chunyu Zhao, Zhenyu Huang, Xudong Luo

In the context of metamaterials, decoupled access to the four constitutive parameters (permittivity, permeability, mass density, and bulk modulus) using a single architecture can unlock substantial design freedom, thereby enabling possibilities for a wide range of electromagnetic and acoustic wave manipulation applications. Herein, we propose a modular replaceable design paradigm for hybrid metamaterials to independently control electromagnetic and acoustic properties within a unified metamaterial unit cell. By arranging printed circuit board traces into an interleaved, meandering lattice, the proposed hybrid metamaterial can simultaneously generate microwave resonances for tuning of negative permittivity and permeability while acting as rigid acoustic boundaries of space-coiled air channels to produce negative mass density and bulk modulus. This hybrid metamaterial is further experimentally demonstrated to realise the simultaneous negative refraction of electromagnetic and acoustic waves. Our design paradigm represents a promising pathway toward advanced hybrid metamaterials, potentially enabling unprecedented functionalities in wave manipulation, sensing, and integrated electromagnetic-acoustic devices.

在超材料的背景下,使用单一架构解耦访问四个本构参数(介电常数、磁导率、质量密度和体积模量)可以解锁大量的设计自由度,从而为广泛的电磁波和声波操纵应用提供了可能性。在此,我们提出了一种模块化的可替换设计范式,用于混合超材料在统一的超材料单元胞内独立控制电磁和声学特性。通过将印刷电路板迹线排列成交错的蜿蜒晶格,所提出的混合超材料可以同时产生微波共振以调谐负介电常数和磁导率,同时作为空间卷曲空气通道的刚性声学边界以产生负质量密度和体积模量。实验进一步证明了这种混合超材料可以同时实现电磁波和声波的负折射。我们的设计范例代表了一条通往先进混合超材料的有希望的途径,可能在波操纵、传感和集成电磁声设备方面实现前所未有的功能。
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引用次数: 0
Scalable and sustainable manufacturing of intermetallic nanocrystals for economical water splitting. 用于经济水分解的可扩展和可持续的金属间纳米晶体制造。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01854d
Mingjin Cui, Haijiao Liu, Ke Chen, Xinwei Shi, Bo Xu, Chenlu Jiang, Dehui Li, Ding Yuan, Yuhai Dou, Chao Wu, Menghao Yang, Shixue Dou, Yu Ding

Intermetallic nanocatalysts are pivotal for advancing energy conversion and storage technologies. However, their industrial-scale synthesis is fundamentally hindered by the difficulty of maintaining precise compositional and structural control. Here, we introduce a universal phase-engineering strategy, actualized through a continuous roll-flow radiative heating platform that enables the one-step, scalable, and controllable synthesis of highly ordered intermetallic nanocatalysts. This innovative technique demonstrates remarkable versatility, rendering precise fabrication of intermetallic nanocrystals across a vast compositional landscape. Crucially, by modulating key kinetic parameters during synthesis, we achieve precise control over ordering arrangement with fine-tuning of catalytic performance. As a proof of concept, we demonstrate the scalable and sustainable synthesis of nickel-iron intermetallic (Ni3Fe) nanocatalysts with a predominant L12-ordered crystal structure for efficient alkaline water splitting. The resulting catalyst exhibits exceptional electrocatalytic activity, reaching a current density of 10 mA cm-2 at a low overpotential of 200.2 mV, a performance that rivals the commercial iridium dioxide (IrO2) benchmark (199.2 mV). Moreover, it shows outstanding long-term durability, with 99.9% current retention over 140 hours and negligible metal leaching. A comprehensive techno-economic evaluation reveals that the hydrogen production cost is strongly dependent on current density, projecting a highly competitive H2 price as low as $2.33 kg-1 at 1.0 A cm-2. This work is expected to provide advanced technology for scalable, sustainable, and continuous manufacturing of intermetallic nanocrystals for economical water splitting.

金属间纳米催化剂是推进能量转换和存储技术的关键。然而,由于难以保持精确的成分和结构控制,它们的工业规模合成从根本上受到阻碍。在这里,我们介绍了一种通用的相工程策略,通过连续滚流辐射加热平台实现了一步,可扩展和可控的高度有序的金属间纳米催化剂合成。这种创新的技术展示了非凡的多功能性,可以在广阔的组成景观中精确地制造金属间纳米晶体。至关重要的是,通过调节合成过程中的关键动力学参数,我们可以通过微调催化性能来精确控制有序排列。作为概念证明,我们展示了可扩展和可持续合成的镍铁金属间化合物(Ni3Fe)纳米催化剂,其主要晶体结构为l12有序,用于高效的碱性水分解。所得到的催化剂表现出优异的电催化活性,在200.2 mV的低过电位下达到10 mA cm-2的电流密度,其性能可与商业二氧化铱(IrO2)基准(199.2 mV)相媲美。此外,它具有出色的长期耐久性,在140小时内保持99.9%的电流,金属浸出可以忽略不计。一项综合技术经济评估显示,氢气生产成本在很大程度上取决于电流密度,预计在1.0 A cm-2下,氢气价格将低至2.33美元/ kg-1,具有很强的竞争力。这项工作有望为可扩展、可持续和连续制造用于经济水分解的金属间纳米晶体提供先进技术。
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引用次数: 0
Construction of hierarchical 2D/2D few-layered MoS2/S-doped g-C3N4 heterojunctions for enhanced photocatalytic formaldehyde removal. 多层2D/2D少层MoS2/ s掺杂g-C3N4异质结的构建增强光催化甲醛去除。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01490e
Yihao Duan, Haihua Wang, Guiqiang Fei, Yu Wang, Liyu Sun

Modification of graphitic carbon nitride (g-C3N4) with semiconductor nanomaterials has been widely investigated as an effective method to enhance its photocatalytic activity. However, the construction of efficient g-C3N4-based heterojunction photocatalysts via an environmentally benign method remains critical. Herein, a two-dimensional (2D) few-layered MoS2/S-doped g-C3N4 hierarchical heterojunction was successfully synthesized by a simple strategy via combining small molecule-assisted liquid exfoliation, calcination and hydrothermal strategy, which was subsequently utilized for photocatalytic formaldehyde removal. The evaluation of the photocatalytic degradation reaction showed that the as-prepared 2D/2D MoS2/S-doped g-C3N4 photocatalysts exhibited superior photocatalytic activity compared to pristine g-C3N4 and S-doped g-C3N4 alone, which was attributed to the intimate interface and rapid charge transfer pathways. This heterojunction structure suppresses the excited electron-hole pair recombination within g-C3N4, which optimally enhances the photodegradation activity owing to high electron-hole pair separation efficiency. The few-layer MoS2 nanosheets play an irreplaceable role due to their unique molybdenum-sulfur atomic arrangement, thereby displaying the superior electronic properties of few-layer or even monolayer nanosheets, which make them an important transfer medium for photoexcited electrons. Meanwhile, S doping effectively modulates the band gap of g-C3N4 and introduces sufficient structural defects to inhibit electron-hole recombination. Moreover, the synthesis employs efficient and non-hazardous reagents, and the resulting catalysts exhibit outstanding stability and recyclability for pollutant degradation.

利用半导体纳米材料对石墨氮化碳(g-C3N4)进行改性是提高其光催化活性的一种有效方法,已被广泛研究。然而,通过环境友好的方法构建高效的g- c3n4基异质结光催化剂仍然是关键。本文采用小分子辅助液体剥离、煅烧和水热相结合的简单策略,成功合成了二维(2D)少层MoS2/ s掺杂g-C3N4层次化异质结,并将其用于光催化甲醛去除。光催化降解反应的评价表明,制备的2D/2D MoS2/ s掺杂g-C3N4光催化剂与原始g-C3N4和单独s掺杂g-C3N4相比,表现出更强的光催化活性,这归因于其紧密的界面和快速的电荷转移途径。这种异质结结构抑制了g-C3N4内部受激发的电子-空穴对复合,从而提高了g-C3N4的光降解活性。少层MoS2纳米片以其独特的钼硫原子排列方式发挥着不可替代的作用,从而显示出少层甚至单层纳米片优越的电子性能,成为光激发电子的重要传递介质。同时,S掺杂有效地调节了g-C3N4的带隙,引入了足够的结构缺陷,抑制了电子-空穴复合。此外,该合成方法采用了高效、无害的试剂,所得到的催化剂具有优异的稳定性和可回收性,可降解污染物。
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Materials Horizons
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