Pub Date : 2025-05-02DOI: 10.1021/acsaem.5c0029510.1021/acsaem.5c00295
Mukilan Muthuramalingam, Kaliyannan Manojkumar, Dhara Sateesh, Arunmetha Sundaramoorthy, Suman Maloji, Chellamuthu Jeganathan, Sugato Hajra, Swati Panda, Hoe Joon Kim, Chella Santhosh* and Venkateswaran Vivekananthan*,
The pressing need for sustainable and efficient energy solutions has spurred considerable advancements in magneto-mechano-electric (MME) generators, which harness the coupling of magnetic, mechanical, and electrical effects to convert ambient energy into electrical power. Unlike traditional energy harvesters, which primarily rely on single transduction mechanisms such as piezoelectric, triboelectric, or electromagnetic effects, MME generators leverage a synergistic approach that integrates magnetostrictive, and piezoelectric effects, enabling superior energy conversion, particularly in low-frequency and low-intensity magnetic environments. This review provides an in-depth analysis of recent progress in MME systems, focusing on key innovations in material development, structural optimization, and hybrid configurations that enhance the energy conversion efficiency. Advances in flexible piezoelectric materials, the integration of magnetostrictive layers for enhanced magnetic responsiveness, and hybrid electromagnetic-piezoelectric systems have expanded the scope of MME applications, particularly in wearable electronics, autonomous sensors, and implantable medical devices. These adaptable generators offer reliable, self-sustaining power for applications such as real-time environmental monitoring, remote IoT sensing, and biocompatible medical technologies while maintaining efficient operation under conditions where conventional harvesters often face performance limitations. By detailing these recent advancements, this review underscores the role of MME technology in enabling decentralized, resilient energy sources, paving the way for the next generation of sustainable power solutions across diverse fields.
{"title":"Beyond Traditional Energy Harvesting: Magneto-Mechano-Electric Technology for Sustainable Powering and Sensing","authors":"Mukilan Muthuramalingam, Kaliyannan Manojkumar, Dhara Sateesh, Arunmetha Sundaramoorthy, Suman Maloji, Chellamuthu Jeganathan, Sugato Hajra, Swati Panda, Hoe Joon Kim, Chella Santhosh* and Venkateswaran Vivekananthan*, ","doi":"10.1021/acsaem.5c0029510.1021/acsaem.5c00295","DOIUrl":"https://doi.org/10.1021/acsaem.5c00295https://doi.org/10.1021/acsaem.5c00295","url":null,"abstract":"<p >The pressing need for sustainable and efficient energy solutions has spurred considerable advancements in magneto-mechano-electric (MME) generators, which harness the coupling of magnetic, mechanical, and electrical effects to convert ambient energy into electrical power. Unlike traditional energy harvesters, which primarily rely on single transduction mechanisms such as piezoelectric, triboelectric, or electromagnetic effects, MME generators leverage a synergistic approach that integrates magnetostrictive, and piezoelectric effects, enabling superior energy conversion, particularly in low-frequency and low-intensity magnetic environments. This review provides an in-depth analysis of recent progress in MME systems, focusing on key innovations in material development, structural optimization, and hybrid configurations that enhance the energy conversion efficiency. Advances in flexible piezoelectric materials, the integration of magnetostrictive layers for enhanced magnetic responsiveness, and hybrid electromagnetic-piezoelectric systems have expanded the scope of MME applications, particularly in wearable electronics, autonomous sensors, and implantable medical devices. These adaptable generators offer reliable, self-sustaining power for applications such as real-time environmental monitoring, remote IoT sensing, and biocompatible medical technologies while maintaining efficient operation under conditions where conventional harvesters often face performance limitations. By detailing these recent advancements, this review underscores the role of MME technology in enabling decentralized, resilient energy sources, paving the way for the next generation of sustainable power solutions across diverse fields.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5513–5543 5513–5543"},"PeriodicalIF":5.4,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934433","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-02DOI: 10.1021/acsaem.5c0061110.1021/acsaem.5c00611
Kevin Bhimani, Apurva Anjan, Varad Mahajani, Rohit M. Manoj and Nikhil Koratkar*,
Metallic aluminum-based aqueous batteries have emerged as promising energy storage devices due to the abundance of metallic aluminum and its high theoretical capacity (gravimetric: 2980 mAh g–1; volumetric: 8056 mAh cm–3). Despite this potential, challenges in the utilization of these batteries arise from the narrow potential window of water and the passivating effects of the high-electrical band gap aluminum oxide (Al2O3) film, hindering the realization of their full potential. A prospective solution involves the development of an electrolyte for aqueous aluminum systems that not only widens the stability window but also effectively removes the passivating oxide layer. In this context, this study investigates the impact of a highly concentrated electrolyte based on Al(ClO4)3 on the performance of an aluminum metal anode. The elevated concentration of the ClO4– anion (maintained via periodic electrolyte replenishment) is found to be highly effective in removing the passivating Al2O3 oxide layer, thereby enabling the facile plating and stripping of aluminum ions from the anode. These findings present a strategic step forward in designing improved electrolytes for aluminum-ion batteries, opening up possibilities for the utilization of aluminum metal anodes in aqueous battery systems.
金属铝基水电池由于其丰富的金属铝和高理论容量(重量:2980 mAh g-1;体积:8056毫安厘米- 3)。尽管具有这种潜力,但由于水的窄电位窗口和高电能带隙氧化铝(Al2O3)膜的钝化作用,阻碍了这些电池的充分潜力的实现,因此在利用这些电池方面存在挑战。一种有前景的解决方案涉及开发一种用于水性铝系统的电解质,这种电解质不仅可以扩大稳定性窗口,还可以有效地去除钝化氧化层。在此背景下,本研究探讨了基于Al(ClO4)3的高浓度电解液对铝金属阳极性能的影响。研究发现,提高ClO4阴离子浓度(通过定期补充电解质来维持)对去除钝化Al2O3氧化层非常有效,从而使阳极上的铝离子易于电镀和剥离。这些发现为设计改进的铝离子电池电解质迈出了战略性的一步,为在水电池系统中使用铝金属阳极开辟了可能性。
{"title":"Tuning the Aluminum–Water Interface in Aqueous Aluminum Metal Batteries","authors":"Kevin Bhimani, Apurva Anjan, Varad Mahajani, Rohit M. Manoj and Nikhil Koratkar*, ","doi":"10.1021/acsaem.5c0061110.1021/acsaem.5c00611","DOIUrl":"https://doi.org/10.1021/acsaem.5c00611https://doi.org/10.1021/acsaem.5c00611","url":null,"abstract":"<p >Metallic aluminum-based aqueous batteries have emerged as promising energy storage devices due to the abundance of metallic aluminum and its high theoretical capacity (gravimetric: 2980 mAh g<sup>–1</sup>; volumetric: 8056 mAh cm<sup>–3</sup>). Despite this potential, challenges in the utilization of these batteries arise from the narrow potential window of water and the passivating effects of the high-electrical band gap aluminum oxide (Al<sub>2</sub>O<sub>3</sub>) film, hindering the realization of their full potential. A prospective solution involves the development of an electrolyte for aqueous aluminum systems that not only widens the stability window but also effectively removes the passivating oxide layer. In this context, this study investigates the impact of a highly concentrated electrolyte based on Al(ClO<sub>4</sub>)<sub>3</sub> on the performance of an aluminum metal anode. The elevated concentration of the ClO<sub>4</sub><sup>–</sup> anion (maintained via periodic electrolyte replenishment) is found to be highly effective in removing the passivating Al<sub>2</sub>O<sub>3</sub> oxide layer, thereby enabling the facile plating and stripping of aluminum ions from the anode. These findings present a strategic step forward in designing improved electrolytes for aluminum-ion batteries, opening up possibilities for the utilization of aluminum metal anodes in aqueous battery systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6194–6202 6194–6202"},"PeriodicalIF":5.4,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934431","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-01DOI: 10.1021/acsaem.5c0083610.1021/acsaem.5c00836
Qingpeng Bao, Zhe Gong, Peng-fei Wang*, Fa-nian Shi and Min Zhu*,
Severe dendrite growth and the process of side reactions have severely affected the application of aqueous zinc-ion batteries (AZIBs) composed of metal zinc anodes in large-scale fields. In this study, basic copper phosphate was synthesized by the hydrothermal method and coated on zinc foil (CUPH-Zn) to solve the above problems. Utilizing the affinity of basic copper phosphate toward zinc, the nucleation resistance was decreased, and the zinc plating/stripping behavior on the surface of the zinc anode was regulated. At the same time, the granular porous morphology formed by freeze-drying is transformed into a nanoflower-shaped porous morphology during the cycling process, which increases the active sites and provides favorable channels for zinc ion deposition. This nanoflower-shaped porous morphology cooperates with the highly hydrophobic basic copper phosphate, inhibits the hydrogen evolution reaction and corrosion reaction, and thereby reduces the formation of byproducts. Owing to these advantages, the CUPH-Zn battery demonstrates outstanding cycle life in both symmetric batteries (Cycle time:700 h, 0.8 mA cm–2 and 13.7% depth of discharge) and full batteries (cycle 3500 times, 2 A g–1 and 3.1 Negative/Positive). Consequently, this study offers innovative insights into constructing a zincophilic and hydrophobic interface layer for highly utilized zinc foil.
严重的枝晶生长和副反应过程严重影响了由金属锌阳极组成的水锌离子电池的大规模应用。为了解决上述问题,本研究采用水热法合成了碱式磷酸铜,并将其涂覆在锌箔上(CUPH-Zn)。利用碱式磷酸铜对锌的亲和力,降低了锌阳极的成核阻力,调节了锌阳极表面的镀锌/剥离行为。同时,通过冷冻干燥形成的颗粒状多孔形态在循环过程中转变为纳米花状多孔形态,增加了活性位点,为锌离子沉积提供了有利的通道。这种纳米花状多孔形态与高疏水性的碱式磷酸铜配合,抑制析氢反应和腐蚀反应,从而减少副产物的形成。由于这些优点,CUPH-Zn电池在对称电池(循环时间:700小时,0.8 mA cm-2和13.7%放电深度)和完全电池(循环3500次,2 A g-1和3.1负/正)中都表现出出色的循环寿命。因此,本研究为构建高利用率锌箔的亲锌疏水界面层提供了创新的见解。
{"title":"Alkaline Copper Phosphate Coating Exhibiting Zincophilic and Hydrophobic Characteristics Achieves High-Performance in Aqueous Zinc-Ion Batteries","authors":"Qingpeng Bao, Zhe Gong, Peng-fei Wang*, Fa-nian Shi and Min Zhu*, ","doi":"10.1021/acsaem.5c0083610.1021/acsaem.5c00836","DOIUrl":"https://doi.org/10.1021/acsaem.5c00836https://doi.org/10.1021/acsaem.5c00836","url":null,"abstract":"<p >Severe dendrite growth and the process of side reactions have severely affected the application of aqueous zinc-ion batteries (AZIBs) composed of metal zinc anodes in large-scale fields. In this study, basic copper phosphate was synthesized by the hydrothermal method and coated on zinc foil (CUPH-Zn) to solve the above problems. Utilizing the affinity of basic copper phosphate toward zinc, the nucleation resistance was decreased, and the zinc plating/stripping behavior on the surface of the zinc anode was regulated. At the same time, the granular porous morphology formed by freeze-drying is transformed into a nanoflower-shaped porous morphology during the cycling process, which increases the active sites and provides favorable channels for zinc ion deposition. This nanoflower-shaped porous morphology cooperates with the highly hydrophobic basic copper phosphate, inhibits the hydrogen evolution reaction and corrosion reaction, and thereby reduces the formation of byproducts. Owing to these advantages, the CUPH-Zn battery demonstrates outstanding cycle life in both symmetric batteries (Cycle time:700 h, 0.8 mA cm<sup>–2</sup> and 13.7% depth of discharge) and full batteries (cycle 3500 times, 2 A g<sup>–1</sup> and 3.1 Negative/Positive). Consequently, this study offers innovative insights into constructing a zincophilic and hydrophobic interface layer for highly utilized zinc foil.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6232–6243 6232–6243"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Transition metal sulfides exhibit superior oxygen evolution reaction electrocatalytic performance due to their unique electronic structures and significant surface reconstructions. The electronic structure of transition metal sulfides can be effectively regulated via heteroatom doping, vacancy engineering, interface engineering, and structure engineering, and surface reconstructions can also be coordinated via coupling with electron-donating carbon materials. Herein, a facile cation regulation strategy is reported to boost the oxygen evolution reaction (OER) activity of transition metal sulfides by pyrolyzing and sulfurizing the Fe2+- and Ni2+-modified ZIF-67 precursor (FeNi/ZIF-67). Crucially, Fe doping and Ni substitution in the final products are achieved by a simple room-temperature ion-exchange strategy, significantly boosting the OER activity. Meanwhile, conductive porous carbon from the organic ligand improves the mass transfer and active-site accessibility. As anticipated, Fe-doped CoS2 and NiCo2S4 embedded in N-doped porous carbon (NC) on carbon cloth (CoFe1Ni2S@NC/CC) demonstrate excellent hydrophilicity and OER activity, representing a very low overpotential of 175 mV at 20 mA cm–2, fast reaction kinetics (Rct = 0.51 Ω cm–2), and considerable electrocatalytic durability in 1.0 M KOH. This work offers a simple and low-cost cation regulation method for designing efficient cobalt-based sulfide hybrid electrocatalysts for OER, advancing their application in electrochemical water splitting.
过渡金属硫化物由于其独特的电子结构和显著的表面重构而表现出优异的析氧反应电催化性能。过渡金属硫化物的电子结构可以通过杂原子掺杂、空位工程、界面工程和结构工程进行有效调控,表面重构也可以通过与供电子碳材料的耦合进行协调。本文报道了一种易阳离子调节策略,通过热解和硫化Fe2+-和Ni2+-修饰的ZIF-67前驱体(FeNi/ZIF-67)来提高过渡金属硫化物的析氧反应(OER)活性。重要的是,最终产物中的Fe掺杂和Ni取代是通过简单的室温离子交换策略实现的,显著提高了OER活性。同时,有机配体的导电多孔碳提高了传质和活性位点的可及性。正如预期的那样,fe掺杂的CoS2和NiCo2S4嵌入在碳布(CoFe1Ni2S@NC/CC)上的n掺杂多孔碳(NC)中,表现出优异的亲水性和OER活性,在20 mA cm-2下具有极低的175 mV过电位,快速的反应动力学(Rct = 0.51 Ω cm-2),并且在1.0 M KOH下具有相当的电催化耐久性。本研究为设计高效的OER钴基硫化物杂化电催化剂提供了一种简单、低成本的阳离子调控方法,促进了其在电化学水分解中的应用。
{"title":"ZIF-67-Derived Cation Regulation of Metal Sulfides for Boosting Oxygen Evolution Activity","authors":"Siwei Guo, Jinhong Wu, Haosen Chen, Ding Huan, Huihua Wang*, Deyong Wang, Dong Hou and Xianglong Li*, ","doi":"10.1021/acsaem.5c0016510.1021/acsaem.5c00165","DOIUrl":"https://doi.org/10.1021/acsaem.5c00165https://doi.org/10.1021/acsaem.5c00165","url":null,"abstract":"<p >Transition metal sulfides exhibit superior oxygen evolution reaction electrocatalytic performance due to their unique electronic structures and significant surface reconstructions. The electronic structure of transition metal sulfides can be effectively regulated via heteroatom doping, vacancy engineering, interface engineering, and structure engineering, and surface reconstructions can also be coordinated via coupling with electron-donating carbon materials. Herein, a facile cation regulation strategy is reported to boost the oxygen evolution reaction (OER) activity of transition metal sulfides by pyrolyzing and sulfurizing the Fe<sup>2+</sup>- and Ni<sup>2+</sup>-modified ZIF-67 precursor (FeNi/ZIF-67). Crucially, Fe doping and Ni substitution in the final products are achieved by a simple room-temperature ion-exchange strategy, significantly boosting the OER activity. Meanwhile, conductive porous carbon from the organic ligand improves the mass transfer and active-site accessibility. As anticipated, Fe-doped CoS<sub>2</sub> and NiCo<sub>2</sub>S<sub>4</sub> embedded in N-doped porous carbon (NC) on carbon cloth (CoFe<sub>1</sub>Ni<sub>2</sub>S@NC/CC) demonstrate excellent hydrophilicity and OER activity, representing a very low overpotential of 175 mV at 20 mA cm<sup>–2</sup>, fast reaction kinetics (<i>R</i><sub>ct</sub> = 0.51 Ω cm<sup>–2</sup>), and considerable electrocatalytic durability in 1.0 M KOH. This work offers a simple and low-cost cation regulation method for designing efficient cobalt-based sulfide hybrid electrocatalysts for OER, advancing their application in electrochemical water splitting.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5770–5780 5770–5780"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934249","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-01DOI: 10.1021/acsaem.5c0020010.1021/acsaem.5c00200
Ziba Rahmati, Nan Wu, Coby Collins, Jiaxin Lu, Morgan Stefik* and Kevin Huang*,
This study investigates a hybrid polymer-ceramic composite electrolyte for solid-state batteries. The polymer is synthesized through the copolymerization of poly(ethylene glycol) methacrylate and poly(methacrylic acid) via the reversible addition–fragmentation chain transfer (RAFT) method followed by postsynthetic functionalization to add phosphonic acid groups, yielding poly(PEGMA-ran-DEPMMA) that can covalently bind to oxide surfaces (Tpoly). The ceramic phase is porous gadolinium-doped cerium oxide (GDC) with a graded porosity made by a phase inversion method. Both monomers in Tpoly interact with anions synergistically for Li-ion conduction. In addition, the binding of phosphonic acid with GDC improves the interfacial stability. A Li symmetric cell with this hybrid electrolyte demonstrated stable performance for over 2000 h at 0.1 mA cm–2 with a critical current density of up to 0.8 mA cm–2. The interfacial resistance of this hybrid electrolyte/Li electrode is reduced by 50% as compared to nontethered PPEGMA. The findings highlight the potential of hybrid polymer-ceramic composites in overcoming interfacial challenges of solid-state lithium-metal battery technology.
研究了一种用于固态电池的聚合物-陶瓷复合电解质。该聚合物是通过可逆加成-裂解链转移(RAFT)法将聚(乙二醇)甲基丙烯酸酯和聚(甲基丙烯酸)共聚合成的,然后通过合成后的功能化加入磷酸基团,得到聚(PEGMA-ran-DEPMMA),该聚(PEGMA-ran-DEPMMA)可以共价结合到氧化物表面(Tpoly)。该陶瓷相为多孔的掺钆氧化铈(GDC),通过相转化法制备了梯度孔隙度。Tpoly中的两种单体与阴离子协同作用以促进锂离子的传导。此外,磷酸与GDC的结合提高了界面的稳定性。在0.1 mA cm-2条件下,锂对称电池的临界电流密度高达0.8 mA cm-2,电池性能稳定超过2000小时。这种混合电解质/锂电极的界面电阻与非系绳PPEGMA相比降低了50%。这一发现突出了混合聚合物-陶瓷复合材料在克服固态锂金属电池技术的界面挑战方面的潜力。
{"title":"Synthesis and Characterization of Tethered Polymer for Hybrid Electrolytes in Solid Lithium-Metal Batteries","authors":"Ziba Rahmati, Nan Wu, Coby Collins, Jiaxin Lu, Morgan Stefik* and Kevin Huang*, ","doi":"10.1021/acsaem.5c0020010.1021/acsaem.5c00200","DOIUrl":"https://doi.org/10.1021/acsaem.5c00200https://doi.org/10.1021/acsaem.5c00200","url":null,"abstract":"<p >This study investigates a hybrid polymer-ceramic composite electrolyte for solid-state batteries. The polymer is synthesized through the copolymerization of poly(ethylene glycol) methacrylate and poly(methacrylic acid) via the reversible addition–fragmentation chain transfer (RAFT) method followed by postsynthetic functionalization to add phosphonic acid groups, yielding poly(PEGMA-<i>ran</i>-DEPMMA) that can covalently bind to oxide surfaces (Tpoly). The ceramic phase is porous gadolinium-doped cerium oxide (GDC) with a graded porosity made by a phase inversion method. Both monomers in Tpoly interact with anions synergistically for Li-ion conduction. In addition, the binding of phosphonic acid with GDC improves the interfacial stability. A Li symmetric cell with this hybrid electrolyte demonstrated stable performance for over 2000 h at 0.1 mA cm<sup>–2</sup> with a critical current density of up to 0.8 mA cm<sup>–2</sup>. The interfacial resistance of this hybrid electrolyte/Li electrode is reduced by 50% as compared to nontethered PPEGMA. The findings highlight the potential of hybrid polymer-ceramic composites in overcoming interfacial challenges of solid-state lithium-metal battery technology.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5800–5810 5800–5810"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrogen, essential for clean and sustainable energy solutions, encounters significant challenges in electrochemical water splitting. This study introduces a Z-Scheme WS2/TiO2 heterostructure synthesized via a hydrothermal method, aimed at enhancing hydrogen evolution reaction (HER) performance through interface engineering. Comprehensive interfacial investigations were conducted by using X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), and UV–vis spectroscopy. XPS analysis revealed peak shifts in the heterostructure, indicative of electronic modifications at the interface. These shifts enhance active site availability, and charge transfer kinetics also corroborated its UPS and UV–vis studies. The establishment of an intimate interface fostering a Z-scheme charge transfer mechanism has been reported. A lower work function of 4.2 eV suggests improved charge transfer at the interface. Furthermore, the development of an internal electric field to achieve Fermi level equilibrium also led to improved HER performance of the Z-scheme-based heterostructure. The prepared heterostructure demonstrated enhanced HER with a lower onset potential (−0.04 V in light and −0.05 V in dark) as compared to pristine WS2 and a lower charge transfer resistance (36.4 Ω in light and 51.2 Ω in dark), highlighting a promising approach for constructing efficient photoelectrochemical device. The study’s insights into strain-induced effects further underscore the potential of the WS2/TiO2 heterostructure for sustainable energy applications. This result paves the way for constructing the facile and efficient method for generating a photoelectrochemical device with solar-to-hydrogen (STH) efficiency equal to 1.16% determined using the water displacement method.
{"title":"Interfacial Engineering of Z-Scheme-Based 2D/1D -WS2/TiO2 Heterostructures: Enhanced Hydrogen Evolution Reaction and Fabrication of Facile Photoelectrochemical Device","authors":"Shivani Dangwal, Saurabh Rawat, Charu Dwivedi, Goutam Kumar Dalapati, Seeram Ramakrishna, Mohit Sharma and Himani Sharma*, ","doi":"10.1021/acsaem.5c0031910.1021/acsaem.5c00319","DOIUrl":"https://doi.org/10.1021/acsaem.5c00319https://doi.org/10.1021/acsaem.5c00319","url":null,"abstract":"<p >Hydrogen, essential for clean and sustainable energy solutions, encounters significant challenges in electrochemical water splitting. This study introduces a Z-Scheme WS<sub>2</sub>/TiO<sub>2</sub> heterostructure synthesized via a hydrothermal method, aimed at enhancing hydrogen evolution reaction (HER) performance through interface engineering. Comprehensive interfacial investigations were conducted by using X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), and UV–vis spectroscopy. XPS analysis revealed peak shifts in the heterostructure, indicative of electronic modifications at the interface. These shifts enhance active site availability, and charge transfer kinetics also corroborated its UPS and UV–vis studies. The establishment of an intimate interface fostering a Z-scheme charge transfer mechanism has been reported. A lower work function of 4.2 eV suggests improved charge transfer at the interface. Furthermore, the development of an internal electric field to achieve Fermi level equilibrium also led to improved HER performance of the Z-scheme-based heterostructure. The prepared heterostructure demonstrated enhanced HER with a lower onset potential (−0.04 V in light and −0.05 V in dark) as compared to pristine WS<sub>2</sub> and a lower charge transfer resistance (36.4 Ω in light and 51.2 Ω in dark), highlighting a promising approach for constructing efficient photoelectrochemical device. The study’s insights into strain-induced effects further underscore the potential of the WS<sub>2</sub>/TiO<sub>2</sub> heterostructure for sustainable energy applications. This result paves the way for constructing the facile and efficient method for generating a photoelectrochemical device with solar-to-hydrogen (STH) efficiency equal to 1.16% determined using the water displacement method.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5911–5924 5911–5924"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Despite the excellent thermoelectric properties of Te, the element diffusion and reaction at the interface with the metal electrodes introduce a large contact resistivity (ρc), significantly reducing the conversion efficiency (η) of the device. Therefore, suitable barrier layers are being sought to optimize the connection between Te and metal electrodes. In this study, a Sn–Te alloy barrier layer is reported based on interfacial reaction. The results indicate that there is no reaction layer or microscopic defects at the interface of the SnTe/Te0.985Sb0.015 device. Additionally, the η of the single-leg device is approximately 4.7% at a temperature difference of 230 K. Notably, this ηmax is 100% higher than that of the Ni/Te0.985Sb0.015/Ni device. Meanwhile, the interface exhibits good thermal stability, with no significant changes observed in ρc, η, and interface microstructure after aging at 523 K for 18 days. This work provides valuable insights into optimizing the interface between thermoelectric materials and metal electrodes, which could lead to the development of more efficient and stable thermoelectric devices.
{"title":"Conversion Efficiency Improvement of Te-Based Thermoelectric Devices through Introduction of the SnTe Alloy Barrier Layer","authors":"Chao Wu, Xin Miao, Aojie Zhang, Mingxing Guo, Jianxiang Lin, Anjun Jin*, Wenhao Fan* and Shaoping Chen*, ","doi":"10.1021/acsaem.5c0073410.1021/acsaem.5c00734","DOIUrl":"https://doi.org/10.1021/acsaem.5c00734https://doi.org/10.1021/acsaem.5c00734","url":null,"abstract":"<p >Despite the e<i>x</i>cellent thermoelectric properties of Te, the element diffusion and reaction at the interface with the metal electrodes introduce a large contact resistivity (<i>ρ</i><sub>c</sub>), significantly reducing the conversion efficiency (<i>η</i>) of the device. Therefore, suitable barrier layers are being sought to optimize the connection between Te and metal electrodes. In this study, a Sn–Te alloy barrier layer is reported based on interfacial reaction. The results indicate that there is no reaction layer or microscopic defects at the interface of the SnTe/Te<sub>0.985</sub>Sb<sub>0.015</sub> device. Additionally, the η of the single-leg device is approximately 4.7% at a temperature difference of 230 K. Notably, this <i>η</i><sub>max</sub> is 100% higher than that of the Ni/Te<sub>0.985</sub>Sb<sub>0.0</sub><sub>15</sub>/Ni device. Meanwhile, the interface exhibits good thermal stability, with no significant changes observed in <i>ρ</i><sub>c</sub>, <i>η</i>, and interface microstructure after aging at 523 K for 18 days. This work provides valuable insights into optimizing the interface between thermoelectric materials and metal electrodes, which could lead to the development of more efficient and stable thermoelectric devices.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6213–6221 6213–6221"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934236","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-01DOI: 10.1021/acsaem.5c0039310.1021/acsaem.5c00393
Yu Rui Wang, Lin Li, Fu Hua Xu, Shuang Li*, Wei Zhang, Yi Xiang Shi and Ningsheng Cai,
An efficient catalyst was studied for the steam reforming reaction of the simulated pyrolysis gas from medical waste (MW) in this paper. The impact of Rh supported on different carrier catalysts on the MW pyrolysis steam reforming performance was investigated. In order to acquire the optimum conditions for hydrogen generation, the impact of reaction temperature, steam/medical waste pyrolysis gas ratio, and gas hourly space velocity on hydrogen production efficiency was studied in the steam reforming reaction. Notably, the reforming and stability performance of 1 wt%Rh/La2Ce2O7 surpassed those of 1 wt%Rh/Al2O3. The former achieved an approximately 60% H2 content and sustained stable hydrogen increment (IH2) and hydrogen selectivity (SH2) values around 520% and 99.5–99.7%, respectively. Moreover, the conversions for C1–C5 (Xi) all exceeded 98%. 1 wt%Rh/La2Ce2O7 has such prominent catalytic performance because H2-TPR and XPS results show that RhOx species were more reducible, and more Rh active species are formed due to strong interaction between Rh and the La2Ce2O7 carrier, which are helpful to the hydrocarbon species adsorption to form intermediate CH* species on Rh metal sites. Besides, the high concentration of oxygen vacancies and active oxygen species on the 1 wt%Rh/La2Ce2O7 catalyst enhanced the adsorption and activation of H2O to form intermediate O*, which facilitates the timely oxidation of intermediate CH* species on the Rh metal surface, ultimately alleviating catalyst surface carbon deposition.
{"title":"La2Ce2O7 Carrier Catalyst for Prominent Steam Reforming Conversion from Medical Waste Pyrolysis Gas to Hydrogen","authors":"Yu Rui Wang, Lin Li, Fu Hua Xu, Shuang Li*, Wei Zhang, Yi Xiang Shi and Ningsheng Cai, ","doi":"10.1021/acsaem.5c0039310.1021/acsaem.5c00393","DOIUrl":"https://doi.org/10.1021/acsaem.5c00393https://doi.org/10.1021/acsaem.5c00393","url":null,"abstract":"<p >An efficient catalyst was studied for the steam reforming reaction of the simulated pyrolysis gas from medical waste (MW) in this paper. The impact of Rh supported on different carrier catalysts on the MW pyrolysis steam reforming performance was investigated. In order to acquire the optimum conditions for hydrogen generation, the impact of reaction temperature, steam/medical waste pyrolysis gas ratio, and gas hourly space velocity on hydrogen production efficiency was studied in the steam reforming reaction. Notably, the reforming and stability performance of 1 wt%Rh/La<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub> surpassed those of 1 wt%Rh/Al<sub>2</sub>O<sub>3</sub>. The former achieved an approximately 60% H<sub>2</sub> content and sustained stable hydrogen increment (<i>I</i><sub>H2</sub>) and hydrogen selectivity (<i>S</i><sub>H2</sub>) values around 520% and 99.5–99.7%, respectively. Moreover, the conversions for C<sub>1</sub>–C<sub>5</sub> (X<sub>i</sub>) all exceeded 98%. 1 wt%Rh/La<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub> has such prominent catalytic performance because H<sub>2</sub>-TPR and XPS results show that RhO<sub><i>x</i></sub> species were more reducible, and more Rh active species are formed due to strong interaction between Rh and the La<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub> carrier, which are helpful to the hydrocarbon species adsorption to form intermediate CH* species on Rh metal sites. Besides, the high concentration of oxygen vacancies and active oxygen species on the 1 wt%Rh/La<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub> catalyst enhanced the adsorption and activation of H<sub>2</sub>O to form intermediate O*, which facilitates the timely oxidation of intermediate CH* species on the Rh metal surface, ultimately alleviating catalyst surface carbon deposition.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5975–5988 5975–5988"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934252","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-01DOI: 10.1021/acsaem.5c0054410.1021/acsaem.5c00544
Iqra Sadiq, Syed Asim Ali* and Tokeer Ahmad*,
In light of heterogeneous catalysis, graphene is the most pivotal allotropic member of the carbon family that has, alongside its derivatives, recently been a part of some of the tremendous benchmarks in energy conversion applications. Graphene derivatives offer imperative ascendancy in photocatalysis for energy conversion on account of their advanced physicochemical characteristics such as enhanced conductivity, surface area, and tunable functionalization. Their role in improving the performance of particulate photocatalysts via one-step excitation paves the way for efficient synthesis of H2, C1, C2 products, and NH3 via photochemical water splitting, CO2 reduction, and N2 fixation processes, respectively. Herein, we present this strategic Review to account for the recent advancements of graphene derivatives in sustainable energy solutions and to inspire researchers to explore the treasure trove of carbon materials. We have articulated progress in the physicochemical properties of graphene derivatives and their experimental touchstones in photochemical water splitting, CO2 reduction, and N2 fixation. Alongside this, the major challenges and prospects related to the applicability of graphene derivatives in these sustainable applications have been presented.
{"title":"Graphene Derivative-Based Particulate Photocatalysts for Energy Conversion Applications: Current Achievements, Bottlenecks, and Future Outlook","authors":"Iqra Sadiq, Syed Asim Ali* and Tokeer Ahmad*, ","doi":"10.1021/acsaem.5c0054410.1021/acsaem.5c00544","DOIUrl":"https://doi.org/10.1021/acsaem.5c00544https://doi.org/10.1021/acsaem.5c00544","url":null,"abstract":"<p >In light of heterogeneous catalysis, graphene is the most pivotal allotropic member of the carbon family that has, alongside its derivatives, recently been a part of some of the tremendous benchmarks in energy conversion applications. Graphene derivatives offer imperative ascendancy in photocatalysis for energy conversion on account of their advanced physicochemical characteristics such as enhanced conductivity, surface area, and tunable functionalization. Their role in improving the performance of particulate photocatalysts via one-step excitation paves the way for efficient synthesis of H<sub>2</sub>, C<sub>1</sub>, C<sub>2</sub> products, and NH<sub>3</sub> via photochemical water splitting, CO<sub>2</sub> reduction, and N<sub>2</sub> fixation processes, respectively. Herein, we present this strategic Review to account for the recent advancements of graphene derivatives in sustainable energy solutions and to inspire researchers to explore the treasure trove of carbon materials. We have articulated progress in the physicochemical properties of graphene derivatives and their experimental touchstones in photochemical water splitting, CO<sub>2</sub> reduction, and N<sub>2</sub> fixation. Alongside this, the major challenges and prospects related to the applicability of graphene derivatives in these sustainable applications have been presented.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5544–5563 5544–5563"},"PeriodicalIF":5.4,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934304","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-30DOI: 10.1021/acsaem.5c0050410.1021/acsaem.5c00504
Xueying Xu, Ziting Liu, Weilin Chen*, Yan Chen, Wenyi He* and Yi Peng*,
Due to the higher electrical conductivity, SnO2 becomes a promising material for electron transport layers (ETLs). However, the mismatched energy level and surface defects lead to unsatisfactory contact between the perovskite film and SnO2 layer, which limits its further application. Herein, heteropoly blue (HPB) r-PMo12–xVx (x = 0, 1, 2) is chosen to modify the interface contact between the perovskite layer and the SnO2 layer. The energy level of HPB-modified SnO2 increases from −4.49 to −4.09 eV, which is more suitable with the perovskite layer, thus improving the electron transport. In addition, the introduction of HPBs reduces the oxygen defects on the surface of SnO2, while metal–oxygen bonding in the HPBs can improve the quality of the perovskite film by passivation. As a result, the photocurrent of the photodetector increases from 22.4 to 81.7 μA, an enhancement of about 3.6 times. In particular, the HPB-modified photodetector can still maintain 90% of the initial performance after 700 h and the stability is significantly improved, providing a good idea for efficient and stable perovskite photodetectors.
{"title":"Heteropoly Blue Modified SnO2 for Highly Efficient Perovskite-Based Photodetectors","authors":"Xueying Xu, Ziting Liu, Weilin Chen*, Yan Chen, Wenyi He* and Yi Peng*, ","doi":"10.1021/acsaem.5c0050410.1021/acsaem.5c00504","DOIUrl":"https://doi.org/10.1021/acsaem.5c00504https://doi.org/10.1021/acsaem.5c00504","url":null,"abstract":"<p >Due to the higher electrical conductivity, SnO<sub>2</sub> becomes a promising material for electron transport layers (ETLs). However, the mismatched energy level and surface defects lead to unsatisfactory contact between the perovskite film and SnO<sub>2</sub> layer, which limits its further application. Herein, heteropoly blue (HPB) r-PMo<sub>12–<i>x</i></sub>V<sub><i>x</i></sub> (<i>x</i> = 0, 1, 2) is chosen to modify the interface contact between the perovskite layer and the SnO<sub>2</sub> layer. The energy level of HPB-modified SnO<sub>2</sub> increases from −4.49 to −4.09 eV, which is more suitable with the perovskite layer, thus improving the electron transport. In addition, the introduction of HPBs reduces the oxygen defects on the surface of SnO<sub>2</sub>, while metal–oxygen bonding in the HPBs can improve the quality of the perovskite film by passivation. As a result, the photocurrent of the photodetector increases from 22.4 to 81.7 μA, an enhancement of about 3.6 times. In particular, the HPB-modified photodetector can still maintain 90% of the initial performance after 700 h and the stability is significantly improved, providing a good idea for efficient and stable perovskite photodetectors.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6112–6120 6112–6120"},"PeriodicalIF":5.4,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934460","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}