Pub Date : 2025-12-25DOI: 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.
{"title":"Advancements and Challenges in Catalytic Nitrogen-to-Ammonia Conversion: Insights into Electrocatalysis, Photocatalysis, and Biocatalysis","authors":"Shih-Mao Peng, , , Muhammad Saukani, , , Chia-Che Chang*, , and , Tsung-Rong Kuo*, ","doi":"10.1021/acsmaterialslett.5c00999","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00999","url":null,"abstract":"<p >Ammonia (NH<sub>3</sub>) 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 CO<sub>2</sub> 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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 2","pages":"334–354"},"PeriodicalIF":8.7,"publicationDate":"2025-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00999","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-24DOI: 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.
{"title":"Regulating Screw Dislocations in Diamond by Tailoring the Chiral Angle of Carbon Nanotube Precursors","authors":"Rong Lin, , , Tao Yu, , , Yanglong Hou*, , and , Shengcai Zhu*, ","doi":"10.1021/acsmaterialslett.5c01405","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01405","url":null,"abstract":"<p >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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 2","pages":"558–566"},"PeriodicalIF":8.7,"publicationDate":"2025-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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.
{"title":"Electrochemically Driven Uranium Capture via Polymer-Based Capacitive Deionization for Radioactive Wastewater Remediation","authors":"Yuting Peng, , , Jiawei Wu, , , ZhangJiashuo Qian, , , Jun Yang, , , Minjie Shi*, , and , Edison Huixiang Ang*, ","doi":"10.1021/acsmaterialslett.5c01345","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01345","url":null,"abstract":"<p >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 UO<sub>2</sub><sup>2+</sup> coordination. In situ characterizations, density functional theory, and molecular dynamics simulations reveal a strong chelation between UO<sub>2</sub><sup>2+</sup> and C═N bonds in the PyHATP lattice, underpinning its selectivity and performance. A proof-of-concept CDI device achieves a record UO<sub>2</sub><sup>2+</sup> adsorption capacity of 676.4 mg g<sup>–1</sup>, 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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 2","pages":"507–516"},"PeriodicalIF":8.7,"publicationDate":"2025-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 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).
{"title":"Oxygen Vacancies Stabilize Zr(III) in the Metal–Organic Framework UiO-66","authors":"Brian G. Diamond, , , Parker S. Brodale, , , Doran L. Pennington, , , Tekalign T. Debela*, , and , Christopher H. Hendon*, ","doi":"10.1021/acsmaterialslett.5c01074","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01074","url":null,"abstract":"<p >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<sup>–7</sup> 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).</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 2","pages":"440–445"},"PeriodicalIF":8.7,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 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。
{"title":"Cation-Dependent Poly(benzimidazobenzophenanthroline):Crown Ether Polymer Blends in n-Type Organic Electrochemical Transistors","authors":"Peter O. Osazuwa, , , Ethan Mackey, , , Cecelia R. Napoli, , , Kelsey P. Koutsoukos, , , Alexa C. Gomez-Taveras, , and , Laure V. Kayser*, ","doi":"10.1021/acsmaterialslett.5c01333","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01333","url":null,"abstract":"<p >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<sup>+</sup>. 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<sup>–3</sup>) compared to NaCl (225 F cm<sup>–3</sup>), and concentration-dependent response toward K<sup>+</sup> over Na<sup>+</sup>, 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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 1","pages":"227–233"},"PeriodicalIF":8.7,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895803","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 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。
{"title":"Surface Induced Order in Room Temperature Ionic Liquids and Its Effect on Piezoelectric Response","authors":"Neelanjana Mukherjee, and , G. J. Blanchard*, ","doi":"10.1021/acsmaterialslett.5c01480","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01480","url":null,"abstract":"<p >We compare the direct piezoelectric response of the room temperature ionic liquid (RTIL) <i>N</i>-butylpyridinium bis(trifluoromethyl-sulfonyl)imide (C<sub>4</sub>Py 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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 2","pages":"609–613"},"PeriodicalIF":8.7,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c01480","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-19DOI: 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.
{"title":"Accessing the Pores and Unlocking Open Metal Sites in a Rare-Earth Cluster-Based Metal–Organic Framework","authors":"Hudson A. Bicalho, , , Clara V. Diniz, , , Zoey Davis, , , Christopher Copeman, , and , Ashlee J. Howarth*, ","doi":"10.1021/acsmaterialslett.5c01391","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01391","url":null,"abstract":"<p >While postsynthetic modification (PSM) of metal–organic frameworks (MOFs) through solvent assisted ligand incorporation (SALI) has been extensively studied, particularly in Zr<sub>6</sub>-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 Y<sub>6</sub>-MOF analogous to Zr-MOF-808 with a 6-connected Y<sub>6</sub>-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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 1","pages":"242–248"},"PeriodicalIF":8.7,"publicationDate":"2025-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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.
{"title":"Recent Advances in MoTe2 Thin Films: Synthesis, Material Properties, and Emerging Applications","authors":"Cuiru Wang, , , Xiongchao Liu, , , Xinyu Li, , , Zhiqiang Yao, , , Wei Hong*, , and , Tifeng Jiao*, ","doi":"10.1021/acsmaterialslett.5c01148","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01148","url":null,"abstract":"<p >MoTe<sub>2</sub>, a notable member of the transition metal dichalcogenides, has attracted significant research interest due to its distinctive properties. This review summarizes recent advances in MoTe<sub>2</sub> 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. MoTe<sub>2</sub> 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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 1","pages":"76–98"},"PeriodicalIF":8.7,"publicationDate":"2025-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-16DOI: 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.
{"title":"Clinically Unmet Needs of Conventional Diabetic Foot Ulcer Dressings","authors":"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*, ","doi":"10.1021/acsmaterialslett.5c00971","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00971","url":null,"abstract":"<p >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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 1","pages":"2–15"},"PeriodicalIF":8.7,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c00971","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-16DOI: 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.
{"title":"Programming Artificial Cells as Bidirectional Genetic Thermometers","authors":"Fan Gao, , , Pawel Jajesniak, , , Xiyan Wang, , , Xiaoqi Wang, , , Yucong Zhou, , , Julien Reboud, , , Baojun Wang*, , and , Jonathan M. Cooper*, ","doi":"10.1021/acsmaterialslett.5c01449","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c01449","url":null,"abstract":"<p >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.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 1","pages":"275–283"},"PeriodicalIF":8.7,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsmaterialslett.5c01449","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}