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Advancements and Challenges in Catalytic Nitrogen-to-Ammonia Conversion: Insights into Electrocatalysis, Photocatalysis, and Biocatalysis 氮-氨催化转化的进展与挑战:对电催化、光催化和生物催化的见解
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-25 DOI: 10.1021/acsmaterialslett.5c00999
Shih-Mao Peng, , , Muhammad Saukani, , , Chia-Che Chang*, , and , Tsung-Rong Kuo*, 

Ammonia (NH3) is vital for modern agriculture and is a potential carbon-free energy carrier. However, its current synthesis via the Haber-Bosch process is energy-intensive, consuming ∼2% of global energy and emitting over 500 Mt of CO2 annually. To address the growing demands for sustainable nitrogen fixation, alternative ammonia synthesis methods under ambient conditions have gained attention. Electrochemical (ENRR), photochemical (PNRR), and biocatalytic (BNRR) nitrogen reduction reactions (NRRs) offer promising approaches. ENRR uses renewable electricity but faces low Faradaic efficiency and competition from hydrogen evolution. PNRR utilizes solar energy but suffers from poor selectivity and low quantum yields. BNRR mimics nitrogenase enzymes with high selectivity but struggles with ATP dependency and scalability. Advances in catalyst design, single-atom engineering, and isotopic validation have improved these strategies, yet challenges remain. This review explores progress, mechanisms, and future directions for sustainable ammonia production.

氨(NH3)对现代农业至关重要,是潜在的无碳能源载体。然而,目前通过Haber-Bosch工艺合成它是能源密集型的,消耗全球能源的2%,每年排放超过5亿吨的二氧化碳。为了满足日益增长的可持续固氮需求,环境条件下替代氨合成方法已引起人们的关注。电化学(ENRR),光化学(PNRR)和生物催化(BNRR)氮还原反应(NRRs)提供了有前途的方法。ENRR使用可再生电力,但面临着低法拉第效率和来自析氢的竞争。PNRR利用太阳能,但选择性差,量子产率低。BNRR具有高选择性,但与ATP依赖性和可扩展性作斗争。催化剂设计、单原子工程和同位素验证的进步改进了这些策略,但挑战仍然存在。本文综述了可持续氨生产的进展、机制和未来发展方向。
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引用次数: 0
Regulating Screw Dislocations in Diamond by Tailoring the Chiral Angle of Carbon Nanotube Precursors 通过调整碳纳米管前体的手性角来调节金刚石中的螺旋位错
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-24 DOI: 10.1021/acsmaterialslett.5c01405
Rong Lin, , , Tao Yu, , , Yanglong Hou*, , and , Shengcai Zhu*, 

Diamond, the hardest natural material, is scarce and expensive to mine, motivating efforts to synthesize high-performance diamond. Dislocations are key microstructural features governing diamond’s mechanical properties, yet their design mechanisms remain unclear. In this work, our large-scale molecular dynamics (MD) simulations demonstrate that the density of screw dislocation in cubic diamond (CD) increases with the increase of chiral angle differences between adjacent graphene layers in multiwalled carbon nanotubes (MWCNTs) during the CNT–diamond phase transition. During the phase transition, larger initial chiral angle differences between adjacent graphene layers increase the zigzag-chain orientation mismatch so that in regions with closely spaced chain intersections the CNT transforms into diamond, whereas in regions with larger mismatch the CNT evolves into screw dislocations. This study reveals the dominant role of the CNT chiral angle in controlling screw dislocations and offers a theoretical framework for improving the performance of synthetic diamond.

金刚石是世界上最坚硬的天然材料,由于开采难度大,开采成本高,因此人们努力合成高性能金刚石。位错是控制金刚石力学性能的关键微观结构特征,但其设计机制尚不清楚。在这项工作中,我们的大规模分子动力学(MD)模拟表明,在多壁碳纳米管(MWCNTs)中,立方金刚石(CD)中的螺旋位错密度随着多壁碳纳米管(MWCNTs)中相邻石墨烯层之间手性角差的增加而增加。在相变过程中,相邻石墨烯层之间较大的初始手性角差增加了之字形链取向错配,因此在链相交紧密的区域,碳纳米管转变为金刚石,而在不匹配较大的区域,碳纳米管演变为螺旋位错。该研究揭示了碳纳米管手性角在控制螺旋位错中的主导作用,为提高合成金刚石的性能提供了理论框架。
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引用次数: 0
Electrochemically Driven Uranium Capture via Polymer-Based Capacitive Deionization for Radioactive Wastewater Remediation 基于聚合物的电容去离子电化学铀捕获技术用于放射性废水的修复
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-23 DOI: 10.1021/acsmaterialslett.5c01345
Yuting Peng, , , Jiawei Wu, , , ZhangJiashuo Qian, , , Jun Yang, , , Minjie Shi*, , and , Edison Huixiang Ang*, 

The removal of uranium(VI) from wastewater is crucial for environmental protection and the development of sustainable nuclear energy. Capacitive deionization (CDI) represents a promising electrochemical strategy, yet its deployment in uranium remediation has been hindered by the absence of efficient electrode materials. Herein, we report a redox-active polymer (PyHATP) electrode that introduces a novel coordination-driven electrochemical extraction concept for highly efficient uranium capture. The π-delocalized framework and abundant redox-active moieties synergistically enhance charge transport and promote reversible UO22+ coordination. In situ characterizations, density functional theory, and molecular dynamics simulations reveal a strong chelation between UO22+ and C═N bonds in the PyHATP lattice, underpinning its selectivity and performance. A proof-of-concept CDI device achieves a record UO22+ adsorption capacity of 676.4 mg g–1, outstanding regeneration stability, and environmental compatibility. In real uranium-contaminated seawater, the system maintains >90% removal efficiency. These findings establish polymer-based CDI as an efficient, selective, and sustainable platform for radioactive wastewater remediation.

废水中铀的脱除对环境保护和核能的可持续发展至关重要。电容去离子(CDI)是一种很有前途的电化学策略,但由于缺乏有效的电极材料,其在铀修复中的应用一直受到阻碍。在此,我们报道了一种氧化还原活性聚合物(PyHATP)电极,该电极引入了一种新的配位驱动的电化学萃取概念,用于高效捕获铀。π-离域框架和丰富的氧化还原活性基团协同增强电荷输运,促进可逆UO22+配位。原位表征、密度泛函理论和分子动力学模拟揭示了PyHATP晶格中UO22+和C = N键之间的强螯合作用,支持了它的选择性和性能。概念验证CDI装置实现了创纪录的676.4 mg g-1的UO22+吸附容量,出色的再生稳定性和环境兼容性。在实际的铀污染海水中,该系统的去除率保持在90%以上。这些发现确立了聚合物基CDI作为一种高效、选择性和可持续的放射性废水修复平台。
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引用次数: 0
Oxygen Vacancies Stabilize Zr(III) in the Metal–Organic Framework UiO-66 金属-有机骨架UiO-66中氧空位稳定Zr(III)
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-22 DOI: 10.1021/acsmaterialslett.5c01074
Brian G. Diamond, , , Parker S. Brodale, , , Doran L. Pennington, , , Tekalign T. Debela*, , and , Christopher H. Hendon*, 

Metal–organic frameworks with a photoaccessible d-manifold are potentially useful for redox catalysis. Yet, electronic structure calculations of materials composed of Zr(IV) preclude the photogeneration of Zr(III). This finding contrasts with a handful of studies that invoke a Zr(III) center in proposed catalytic cycles. Defects may be responsible for stabilizing Zr(III) centers. Here we examine the effects of hydrogenic and oxygenic defects on the position of the band edges in a representative Zr(IV)-containing framework, UiO-66. While Brønsted acid/base-type defects are generally favorable, none yield a Zr d-state below the computational hydrogen evolution reaction (HER). However, oxygenic vacancies may stabilize a Zr d-orbital ∼0.5 eV below the HER. The oxygenic defect occurs with a formation energy of +2.3 eV, and concentration of 1.50 × 10–7 defects/mol at 373 K of Zr(III), essentially preventing the defect without alternative stabilization. If such vacancies were installed, they may be the origin of Zr(III).

具有光可达d流形的金属有机骨架在氧化还原催化中具有潜在的用途。然而,由Zr(IV)组成的材料的电子结构计算排除了Zr(III)的光生。这一发现与少数在提出的催化循环中调用Zr(III)中心的研究形成对比。缺陷可能是稳定Zr(III)中心的原因。在这里,我们研究了氢缺陷和氧缺陷对具有代表性的含Zr(IV)框架UiO-66的能带边缘位置的影响。虽然Brønsted酸/碱型缺陷通常是有利的,但没有一个能产生低于计算析氢反应(HER)的Zr d态。然而,氧空位可以使Zr d轨道稳定在HER以下~ 0.5 eV。氧化缺陷的形成能为+2.3 eV, Zr(III)浓度为1.50 × 10-7个缺陷/mol,在373 K Zr(III)下发生,基本上防止了缺陷的发生,没有替代稳定。如果安装了这样的空位,它们可能是Zr(III)的来源。
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引用次数: 0
Cation-Dependent Poly(benzimidazobenzophenanthroline):Crown Ether Polymer Blends in n-Type Organic Electrochemical Transistors 阳离子依赖性聚苯并咪唑苯并菲罗啉:冠醚聚合物共混物在n型有机电化学晶体管中的应用
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-22 DOI: 10.1021/acsmaterialslett.5c01333
Peter O. Osazuwa, , , Ethan Mackey, , , Cecelia R. Napoli, , , Kelsey P. Koutsoukos, , , Alexa C. Gomez-Taveras, , and , Laure V. Kayser*, 

N-type organic electrochemical transistors (OECTs) hold promise for cation-responsive bioelectronics; however, their application in this area lags behind that of their p-type counterparts. Here, we introduce a BBL:PVB18C6 polymer blend synthesized via acid-mediated in situ polymerization of vinylbenzo-18-crown-6 (VB18C6) in the presence of poly(benzimidazobenzophenanthroline) (BBL) in methanesulfonic acid, enabling homogeneous integration of crown ether motifs selective for K+. Quantitative integration of the X-ray photoemission spectra provided direct evidence of differential cation uptake in BBL and BBL:PVB18C6, underscoring the cation recognition capability of the polymer blend. When employed as the channel in OECTs, BBL:PVB18C6 devices exhibit enhanced drain current, 76% higher volumetric capacitance in KCl (395 F cm–3) compared to NaCl (225 F cm–3), and concentration-dependent response toward K+ over Na+, while retaining excellent operational stability. This work establishes a strategy for functionalizing BBL with ion-selective motifs, enabling the development of cation-dependent n-type OECTs.

n型有机电化学晶体管(OECTs)有望用于阳离子响应生物电子学;然而,它们在这一领域的应用落后于p型同行。在此,我们介绍了一种BBL:PVB18C6聚合物共混物,在甲磺酸中,在聚苯并咪唑苯并菲罗啉(BBL)存在的情况下,通过酸介导的原位聚合,合成了乙烯基苯并-18-冠-6 (VB18C6),使冠醚基序具有选择性K+的均匀整合。x射线光发射光谱的定量积分提供了BBL和BBL:PVB18C6中阳离子摄取差异的直接证据,强调了聚合物共混物的阳离子识别能力。当BBL:PVB18C6器件用作oect中的通道时,其漏极电流增强,在KCl (395 F cm-3)中的体积电容比NaCl (225 F cm-3)高76%,并且对K+的响应与浓度相关,而不是Na+,同时保持了优异的工作稳定性。这项工作建立了一个用离子选择性基序功能化BBL的策略,使阳离子依赖的n型oect得以发展。
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引用次数: 0
Surface Induced Order in Room Temperature Ionic Liquids and Its Effect on Piezoelectric Response 室温离子液体表面诱导有序及其对压电响应的影响
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-22 DOI: 10.1021/acsmaterialslett.5c01480
Neelanjana Mukherjee,  and , G. J. Blanchard*, 

We compare the direct piezoelectric response of the room temperature ionic liquid (RTIL) N-butylpyridinium bis(trifluoromethyl-sulfonyl)imide (C4Py TFSI) under conditions where pressure is applied to the bulk RTIL in a vessel with a bare ITO interface and a vessel with an ITO interface modified with a monolayer of a pyridinium-containing amphiphile. We find that the presence of a single monolayer of the pyridinium amphiphile poises the RTIL structurally to produce a measurably larger piezoelectric response. The extent of order imposed by the presence of the monolayer is likely limited by the intrinsic surface roughness and structural irregularity of the ITO-coated glass support used.

我们比较了室温离子液体(RTIL) n -丁基吡啶双(三氟甲基磺酰基)亚胺(C4Py TFSI)在具有裸ITO界面的容器和具有单层含吡啶两亲性修饰的ITO界面的容器中施加压力的条件下的直接压电响应。我们发现,单层吡啶两亲体的存在使RTIL在结构上产生可测量的更大的压电响应。单分子层的存在所施加的有序程度很可能受到所使用的ito涂层玻璃支架的固有表面粗糙度和结构不规则性的限制。
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引用次数: 0
Accessing the Pores and Unlocking Open Metal Sites in a Rare-Earth Cluster-Based Metal–Organic Framework 基于稀土团簇的金属有机骨架中孔隙的获取和开放金属位的解锁
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-19 DOI: 10.1021/acsmaterialslett.5c01391
Hudson A. Bicalho, , , Clara V. Diniz, , , Zoey Davis, , , Christopher Copeman, , and , Ashlee J. Howarth*, 

While postsynthetic modification (PSM) of metal–organic frameworks (MOFs) through solvent assisted ligand incorporation (SALI) has been extensively studied, particularly in Zr6-based MOFs, this PSM approach is largely overlooked in the literature on rare-earth (RE) cluster-based MOFs. In this work, we explore SALI in Y-CU-45 (CU = Concordia University), a Y6-MOF analogous to Zr-MOF-808 with a 6-connected Y6-node. The structural connectivity of Y-CU-45 allows for the existence of six coordinatively unsaturated sites per cluster. We previously demonstrated that these sites are capped by modulators used in the synthesis of Y-CU-45, which partially occlude the pores of the MOF. By performing SALI on Y-CU-45 with seven different ligands: formate, acetate, trifluoroacetate, pivalate, benzoate, 2,3,4,5-tetrafluorobenzoate, and 2,6-bis(trifluoromethyl)benzoate, we demonstrate that the pores and open metal sites of Y-CU-45 can be made more accessible.

虽然通过溶剂辅助配体掺入(SALI)对金属有机骨架(mof)进行合成后修饰(PSM)已经得到了广泛的研究,特别是在基于zr6的mof中,但这种PSM方法在基于稀土(RE)簇的mof的文献中很大程度上被忽视了。在这项工作中,我们探索了Y-CU-45 (CU = Concordia University)中的SALI,这是一种类似于Zr-MOF-808的Y6-MOF,具有6连接的y6节点。Y-CU-45的结构连通性允许每个簇存在六个协调不饱和位点。我们之前证明了这些位点被用于Y-CU-45合成的调制剂所覆盖,这些调制剂部分阻塞了MOF的孔隙。通过用甲酸酯、乙酸酯、三氟乙酸酯、戊酸酯、苯甲酸酯、2,3,4,5-四氟苯甲酸酯和2,6-二(三氟甲基)苯甲酸酯等七种不同的配体对Y-CU-45进行SALI,我们证明Y-CU-45的孔和开放的金属位点可以更容易接近。
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引用次数: 0
Recent Advances in MoTe2 Thin Films: Synthesis, Material Properties, and Emerging Applications MoTe2薄膜的最新进展:合成、材料性能和新兴应用
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1021/acsmaterialslett.5c01148
Cuiru Wang, , , Xiongchao Liu, , , Xinyu Li, , , Zhiqiang Yao, , , Wei Hong*, , and , Tifeng Jiao*, 

MoTe2, a notable member of the transition metal dichalcogenides, has attracted significant research interest due to its distinctive properties. This review summarizes recent advances in MoTe2 thin films, focusing on their properties, synthesis, and applications. We first discuss the structure–property relationships, particularly how crystal structure influences electronic, optical, and transport properties, along with environmental stability. Various synthesis methods are examined, including mechanical exfoliation, chemical vapor deposition, molecular beam epitaxy, solution-phase exfoliation, and wet-chemical approaches, as well as postsynthesis phase engineering techniques. MoTe2 demonstrates considerable potential in rigid and flexible electronics, optoelectronics, electrochemical energy storage, hydrogen evolution reaction catalysis, and quantum devices. However, challenges remain in achieving large-scale, high-quality, phase-controllable films with improved stability. Future research should prioritize synthesis optimization, performance enhancement, and exploration of novel functionalities for next-generation technologies.

MoTe2是过渡金属二硫族化合物中重要的一员,由于其独特的性质引起了人们的极大兴趣。本文综述了近年来MoTe2薄膜的研究进展,重点介绍了MoTe2薄膜的性质、合成和应用。我们首先讨论了结构-性质关系,特别是晶体结构如何影响电子、光学和输运性质,以及环境稳定性。研究了各种合成方法,包括机械剥落、化学气相沉积、分子束外延、液相剥落、湿化学方法以及合成后相工程技术。MoTe2在刚性和柔性电子学、光电子学、电化学储能、析氢反应催化和量子器件方面显示出相当大的潜力。然而,在实现具有更高稳定性的大规模、高质量、相位可控薄膜方面仍然存在挑战。未来的研究应优先考虑合成优化、性能增强和探索下一代技术的新功能。
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引用次数: 0
Clinically Unmet Needs of Conventional Diabetic Foot Ulcer Dressings 常规糖尿病足溃疡敷料的临床未满足需求
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-16 DOI: 10.1021/acsmaterialslett.5c00971
Chung-Wei Roy Hsu, , , Hien A. Tran, , , Kieran Lau*, , , Yiwei Li, , , Minh Hieu Ho, , , Yu Shrike Zhang, , , Brooke L. Farrugia, , , Steven G. Wise, , , Jelena Rnjak-Kovacina, , , Tiziano Serra, , , Elena M. De-Juan-Pardo, , , Shirley J. Jansen, , and , Khoon S. Lim*, 

Diabetic foot ulcers (DFUs) represent one of the most complex and challenging chronic wounds to manage, carrying a high risk of limb amputation due to the multifactorial comorbidities of hyperglycemia, including peripheral neuropathy, arterial occlusive disease, and immune dysfunction. The current clinical gold standard treatment for DFUs involves surgical debridement, followed by the application of appropriate wound dressings. Although numerous commercial products are available and advanced dressings are currently in research development and clinical trials, most still fail to meet the clinical criteria for an ideal dressing. This Perspective highlights the current focus of DFU wound dressing research and identifies key translational gaps. These include the reliance on oversimplified validation models, the tendency to address only one or two pathological features (e.g., infection or angiogenesis), and limited consideration of dressing and other management needs in post-amputation care. We thenpropose the ideal properties required for the development of proactive, multifunctional, and smart wound dressings that can address a broader spectrum of DFU pathophysiologies. Furthermore, we emphasize that such designs should also prioritize simplicity and manufacturability to meet regulatory requirements and facilitate clinical translation.

糖尿病足溃疡(DFUs)是最复杂和最具挑战性的慢性伤口之一,由于高血糖的多因素合并症,包括周围神经病变、动脉闭塞性疾病和免疫功能障碍,具有截肢的高风险。目前临床治疗DFUs的金标准包括手术清创,然后应用适当的伤口敷料。尽管有许多商业产品可供使用,先进的敷料目前正在研究开发和临床试验中,但大多数仍然不能满足理想敷料的临床标准。本展望强调了目前DFU伤口敷料研究的重点,并确定了关键的翻译差距。这些问题包括依赖过于简化的验证模型,倾向于只处理一两个病理特征(例如,感染或血管生成),以及在截肢后护理中对包扎和其他管理需求的考虑有限。然后,我们提出了开发主动性,多功能和智能伤口敷料所需的理想特性,可以解决更广泛的DFU病理生理问题。此外,我们强调这种设计还应优先考虑简单性和可制造性,以满足法规要求并促进临床翻译。
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引用次数: 0
Programming Artificial Cells as Bidirectional Genetic Thermometers 编程人工细胞作为双向遗传温度计
IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-16 DOI: 10.1021/acsmaterialslett.5c01449
Fan Gao, , , Pawel Jajesniak, , , Xiyan Wang, , , Xiaoqi Wang, , , Yucong Zhou, , , Julien Reboud, , , Baojun Wang*, , and , Jonathan M. Cooper*, 

Cell-free protein synthesis (CFPS) systems offer a powerful platform for engineering synthetic gene circuits with rapid prototyping and modular control. Using this technique, artificial cells have been produced for a range of biomedical applications, such as biosensing, drug delivery, and tissue engineering. However, associated regulatory strategies rely predominantly on chemical induction, lacking the spatiotemporal precision required for clinical translation. Here, we engineer a bidirectional genetic thermometer using the TlpA transcriptional regulator, achieving bidirectional thermal regulation in both CFPS and artificial cells. Counter to its canonical role as a high-temperature regulator in living systems, TlpA exhibited temperature-dependent activation and repression in CFPS, enabling programmable gene expression across discrete thermal thresholds. Our bidirectional thermometers were integrated into alginate microbeads, creating functional thermal microsensors on a path toward smart thermal materials. This work establishes a bidirectional temperature control system for artificial cells and offers insights into the integration of genetic circuits with biomaterial engineering.

无细胞蛋白合成(CFPS)系统为工程合成基因电路提供了一个强大的平台,具有快速原型和模块化控制。利用这一技术,人造细胞已被用于一系列生物医学应用,如生物传感、药物输送和组织工程。然而,相关的调控策略主要依赖于化学诱导,缺乏临床转化所需的时空精度。在这里,我们使用TlpA转录调节因子设计了一个双向遗传温度计,实现了CFPS和人工细胞的双向热调节。与TlpA在生命系统中作为高温调节器的典型作用相反,TlpA在CFPS中表现出温度依赖性的激活和抑制,使可编程基因在离散的热阈值上表达。我们的双向温度计被集成到海藻酸盐微珠中,在智能热材料的道路上创造了功能性热微传感器。本研究建立了人工细胞的双向温度控制系统,为遗传电路与生物材料工程的整合提供了新的思路。
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引用次数: 0
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