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Efficiency in photocatalytic production of hydrogen: energetic and sustainability implications 光催化制氢的效率:能源和可持续性影响
IF 3.2
Energy advances Pub Date : 2024-09-02 DOI: 10.1039/D4YA00361F
Rocío Sayago-Carro, Luis José Jiménez-Chavarriga, Esperanza Fernández-García, Anna Kubacka and Marcos Fernández-García
{"title":"Efficiency in photocatalytic production of hydrogen: energetic and sustainability implications","authors":"Rocío Sayago-Carro, Luis José Jiménez-Chavarriga, Esperanza Fernández-García, Anna Kubacka and Marcos Fernández-García","doi":"10.1039/D4YA00361F","DOIUrl":"10.1039/D4YA00361F","url":null,"abstract":"<p >Hydrogen generation through a photocatalytic process appears to be a promising technology to produce this energy vector through a novel, efficient, green, and sustainable process. The fruitful use of sunlight as an excitation source and renewable bio-derived reactants as well as the development of highly efficient catalysts are required to achieve this goal. In this perspective article, we focus on describing how to braid energy and sustainability sides of hydrogen photo-generation into a single parameter, allowing quantitative measurement and trustful comparison of different catalytic systems. Starting from the energy-related efficiency parameters defined by the IUPAC, we present novel approaches leading to parameters enclosing energy and sustainability information. The study is completed with the analysis of other, non-IUPAC, parameters of broad use such as the solar-to-hydrogen observable. The set of results available in the literature for the water splitting reaction and the use of bio-derived sacrificial molecules are reviewed to assess the potential of such reactions in the energy-efficient and sustainable production of hydrogen.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 11","pages":" 2738-2757"},"PeriodicalIF":3.2,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00361f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correction: Acid–base concentration swing for direct air capture of carbon dioxide 更正:直接空气捕集二氧化碳的酸碱浓度摆动
IF 3.2
Energy advances Pub Date : 2024-08-30 DOI: 10.1039/D4YA90035A
Anatoly Rinberg and Michael J. Aziz
{"title":"Correction: Acid–base concentration swing for direct air capture of carbon dioxide","authors":"Anatoly Rinberg and Michael J. Aziz","doi":"10.1039/D4YA90035A","DOIUrl":"https://doi.org/10.1039/D4YA90035A","url":null,"abstract":"<p >Correction for ‘Acid–base concentration swing for direct air capture of carbon dioxide’ by Anatoly Rinberg and Michael J. Aziz, <em>Energy Adv.</em>, 2024, https://doi.org/10.1039/d4ya00251b.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 2416-2416"},"PeriodicalIF":3.2,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya90035a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142174073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Anion exchange membrane water electrolysis over superparamagnetic ferrites† 超顺磁性铁氧体上的阴离子交换膜电解水
IF 3.2
Energy advances Pub Date : 2024-08-30 DOI: 10.1039/D4YA00170B
Tiago Fernandes, Ramsundar Rani Mohan, Laura Donk, Wei Chen, Chiara Biz, Mauro Fianchini, Saeed Kamali, Siavash Mohammad Alizadeh, Anna Kitayev, Aviv Ashdot, Miles Page, Laura M. Salonen, Sebastian Kopp, Ervin Tal Gutelmacher, José Gracia, Marta Costa Figueiredo and Yury V. Kolen’ko
{"title":"Anion exchange membrane water electrolysis over superparamagnetic ferrites†","authors":"Tiago Fernandes, Ramsundar Rani Mohan, Laura Donk, Wei Chen, Chiara Biz, Mauro Fianchini, Saeed Kamali, Siavash Mohammad Alizadeh, Anna Kitayev, Aviv Ashdot, Miles Page, Laura M. Salonen, Sebastian Kopp, Ervin Tal Gutelmacher, José Gracia, Marta Costa Figueiredo and Yury V. Kolen’ko","doi":"10.1039/D4YA00170B","DOIUrl":"10.1039/D4YA00170B","url":null,"abstract":"<p >The oxygen evolution reaction (OER) is usually the bottleneck in water electrolysis due to its sluggish kinetics, resulting in increased costs in the production of green hydrogen. Therefore, there is a need for more efficient, stable, and ideally, critical-raw-material-free catalysts. To this end, we have synthesized nanosized spinel ferrites CoFe<small><sub>2</sub></small>O<small><sub>4</sub></small>, NiFe<small><sub>2</sub></small>O<small><sub>4</sub></small>, and ZnFe<small><sub>2</sub></small>O<small><sub>4</sub></small>, and a high-entropy spinel ferrite Zn<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>2.2</sub></small>O<small><sub>4</sub></small> through a simple coprecipitation reaction in an automated reactor on a gram scale. The powder X-ray diffraction and transmission electron microscopy studies revealed crystallite sizes of 20–35 nm. Insight into the oxidation states and cation distribution in the mixed spinel systems was gained through X-ray photoelectron and Mössbauer spectroscopy studies. The activity of all spinel ferrites was tested for the OER through half-cell laboratory measurements and full-cell anion exchange membrane electrolysis (AEMEL), where Zn<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>2.2</sub></small>O<small><sub>4</sub></small> showed the lowest overpotential of 432 mV at a current density of 10 mA cm<small><sup>−2</sup></small>. All the synthesized ferrites demonstrated good stability up to 20 h, with NiFe<small><sub>2</sub></small>O<small><sub>4</sub></small> being the most active in high current density experiments up to 2 A cm<small><sup>−2</sup></small>. In addition, studies on the magnetic properties at room temperature revealed a largely superparamagnetic response of the prepared materials, indicating that quantum spin-exchange interactions facilitate oxygen electrochemistry. Computational calculations shed light on the superior catalytic activities of NiFe<small><sub>2</sub></small>O<small><sub>4</sub></small> and Zn<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>2.2</sub></small>O<small><sub>4</sub></small>, the two strongly correlated oxides that exhibit the highest magnetization and the smallest band gaps, corroborating the recent principles determining the activity of magnetic oxides in electron transfer reactions.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 2575-2586"},"PeriodicalIF":3.2,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00170b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Direct formate anion exchange membrane fuel cells with a PdAu bimetallic nanoparticle anode electrocatalyst obtained by metal vapor synthesis† 采用通过金属蒸气合成获得的 PdAu 双金属纳米粒子阳极电催化剂的直接甲酸阴离子交换膜燃料电池
IF 3.2
Energy advances Pub Date : 2024-08-29 DOI: 10.1039/D4YA00324A
Carolina Castello, Tailor Peruzzolo, Marco Bellini, Maria V. Pagliaro, Francesco Bartoli, Enrico Berretti, Lorenzo Poggini, Emanuela Pitzalis, Claudio Evangelisti and Hamish A. Miller
{"title":"Direct formate anion exchange membrane fuel cells with a PdAu bimetallic nanoparticle anode electrocatalyst obtained by metal vapor synthesis†","authors":"Carolina Castello, Tailor Peruzzolo, Marco Bellini, Maria V. Pagliaro, Francesco Bartoli, Enrico Berretti, Lorenzo Poggini, Emanuela Pitzalis, Claudio Evangelisti and Hamish A. Miller","doi":"10.1039/D4YA00324A","DOIUrl":"10.1039/D4YA00324A","url":null,"abstract":"<p >Fuels can be produced from the electrochemical reduction of industrial waste CO<small><sub>2</sub></small> (e-fuels) using renewable energy and hence are an attractive option for the storage of renewable energy in a chemical form. The energy stored in the e-Fuel may be recovered on-demand using a direct fuel cell thus completing a carbon neutral cycle. Anion exchange membrane fuel cells (AEMFCs) are versatile devices that can be fed by both a gaseous fuel such as H<small><sub>2</sub></small> and with liquid fuels (<em>e.g.</em> alcohols, formate, hydrazine, NaBH<small><sub>4</sub></small>). Formate is a molecule that can be easily obtained by the electrochemical reduction of CO<small><sub>2</sub></small> with high selectivity. Efficient re-transformation of the energy stored in the chemical bonds into electrical energy requires the development of efficient and stable electrocatalysts. Palladium alloy catalysts are highly active under alkaline conditions when Pd is mixed with more oxophilic transition metals. Here we report that enhanced activity and stability can be obtained with Au–Pd alloy nanoparticles when compared to a Pd catalyst. Both catalysts are prepared by a metal vapour synthesis method. We show that the key to enhanced performance is the partial segregation of Au to the NP surface that increases oxophilicity and favours the adsorption and transfer of OH<small><sup>−</sup></small> species to the active Pd sites. This enhanced activity translates to high power densities and performance stability when employed in AEMFCs fed with aqueous potassium formate fuel (Peak power density of 0.14 W cm<small><sup>−2</sup></small>, energy efficiency of 33%, faradaic efficiency of 80%).</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 2520-2529"},"PeriodicalIF":3.2,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00324a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Quantitative local state of charge mapping by operando electrochemical fluorescence microscopy in porous electrodes† 通过多孔电极中的操作电化学荧光显微镜绘制定量局部电荷状态图
IF 3.2
Energy advances Pub Date : 2024-08-28 DOI: 10.1039/D4YA00362D
Anton M. Graf, Thomas Cochard, Kiana Amini, Michael S. Emanuel, Shmuel M. Rubinstein and Michael J. Aziz
{"title":"Quantitative local state of charge mapping by operando electrochemical fluorescence microscopy in porous electrodes†","authors":"Anton M. Graf, Thomas Cochard, Kiana Amini, Michael S. Emanuel, Shmuel M. Rubinstein and Michael J. Aziz","doi":"10.1039/D4YA00362D","DOIUrl":"10.1039/D4YA00362D","url":null,"abstract":"<p >We introduce <em>operando</em> quantitative electrochemical fluorescence state of charge mapping (QEFSM), a non-invasive technique to study operating electrochemical systems along with a new design of optically transparent microfluidic redox flow cells compatible with the most demanding optical requirements. QEFSM allows quantitative mappings of the concentration of a particular oxidation state of a redox-active species within a porous electrode during its operation. In this study, we used confocal microscopy to map the fluorescence signal of the reduced form of 2,7-anthraquinone disulfonate (AQDS) in a set of multistep-chronoamperometry experiments. Calibrating these images and incorporating an analytical model of quinhydrone heterodimer formation with no free parameters, and accounting for the emission of each species involved, we determined the local molecular concentration and the state of charge (SOC) fields within a commercial porous electrode during operation. With this method, electrochemical conversion and species advection, reaction and diffusion can be monitored at heretofore unprecedented transverse and axial resolution (1 μm and 25 μm, respectively) at frame rates of 0.5 Hz, opening new routes to understanding local electrochemical processes in porous electrodes. We observed pore-scale SOC inhomogeneities appearing when the fraction of electroactive species converted in a single pass through the electrode becomes large.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 2468-2478"},"PeriodicalIF":3.2,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00362d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ion-conductive vs. non-ion-conductive ceramic fillers in silane-linked polyethylene oxide-based composite polymer electrolytes with high room-temperature ionic conductivity† 具有高室温离子导电性的硅烷连接聚乙烯氧化物基复合聚合物电解质中的离子导电与非离子导电陶瓷填料
IF 3.2
Energy advances Pub Date : 2024-08-28 DOI: 10.1039/D4YA00231H
Eun Ju Jeon, Sharif Haidar, Laura Helmers, Arno Kwade and Georg Garnweitner
{"title":"Ion-conductive vs. non-ion-conductive ceramic fillers in silane-linked polyethylene oxide-based composite polymer electrolytes with high room-temperature ionic conductivity†","authors":"Eun Ju Jeon, Sharif Haidar, Laura Helmers, Arno Kwade and Georg Garnweitner","doi":"10.1039/D4YA00231H","DOIUrl":"10.1039/D4YA00231H","url":null,"abstract":"<p >Polyethylene oxide (PEO)-based polymer electrolytes, despite their cost-effectiveness and ease of processing, suffer from low ionic conductivity at lower temperatures due to the semi-crystalline nature of PEO. Incorporating ceramic filler particles into the polymer matrix offers a potential solution by disrupting its rigid crystalline structure, thereby improving the flexibility of the polymer chains. However, the Li ion conduction pathway within these composite polymer electrolytes (CPEs) remains predominantly within the polymer matrix if the filler particles are only physically mixed. The surface modification of filler particles can improve the interfacial compatibility and ionic conductivity. In this work, two types of filler particles, passive ZrO<small><sub>2</sub></small> and active Li<small><sub>7</sub></small>La<small><sub>3</sub></small>Zr<small><sub>2</sub></small>O<small><sub>12</sub></small> (LLZO), are compared and incorporated into PEO–polyethylene glycol (PEG)–lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) CPEs. The surface of the filler particles is functionalized with a silane ligand ((3-glycidyloxypropyl)trimethoxysilane (GPTMS)) prior to their integration into the PEO matrix. This modifies the interfacial properties between the polymer and the filler particles, hence influencing the ionic conductivity. The functionalized ZrO<small><sub>2</sub></small> fillers enhance the ionic conductivity of the CPEs by reducing the crystallinity of PEO. The PEO–PEG–LiTFSI CPE with 15 vol% of GPTMS–ZrO<small><sub>2</sub></small> achieved an ionic conductivity of 6.66 × 10<small><sup>−4</sup></small> S cm<small><sup>−1</sup></small> at 20 °C, which is significantly higher than that of the standard PEO–LiTFSI (9.26 × 10<small><sup>−6</sup></small> S cm<small><sup>−1</sup></small>). Additionally, coupling GPTMS to PEO chains without the introduction of filler particles also improved the ionic conductivity, while the incorporation of functionalized LLZO fillers does not, which is attributed to a LiCO<small><sub>3</sub></small> passivation layer. The results suggest a viable strategy to overcome the inherent limitations of PEO electrolyte, thus offering valuable insights into the design and optimization of CPEs for practical applications.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 2428-2438"},"PeriodicalIF":3.2,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00231h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optical constants manipulation of formamidinium lead iodide perovskites: ellipsometric and spectroscopic twigging† 操纵甲脒碘化铅包晶石的光学常数:椭偏和光谱分析。
IF 3.2
Energy advances Pub Date : 2024-08-26 DOI: 10.1039/D4YA00339J
Mohd Taukeer Khan, Muhammed P. U. Haris, Baraa Alhouri, Samrana Kazim and Shahzada Ahmad
{"title":"Optical constants manipulation of formamidinium lead iodide perovskites: ellipsometric and spectroscopic twigging†","authors":"Mohd Taukeer Khan, Muhammed P. U. Haris, Baraa Alhouri, Samrana Kazim and Shahzada Ahmad","doi":"10.1039/D4YA00339J","DOIUrl":"10.1039/D4YA00339J","url":null,"abstract":"<p >Unraveling the knowledge of the complex refractive index and photophysical properties of the perovskite layer is paramount to uncovering the physical process that occurs in a perovskite solar cell under illumination. Herein, we probed the optical and photophysical properties of FAPbI<small><sub>3</sub></small> (FAPI) and Cs<small><sub>0.1</sub></small>FA<small><sub>0.9</sub></small>PbI<small><sub>3</sub></small> (CsFAPI) thin films deposited from pre-synthesized powder, by the spectroscopic ellipsometer and time-resolved fluorescence spectra. We determined the complex refractive index of perovskite films by fitting the measured spectroscopic ellipsometer data with the three-oscillator Tauc–Lorentz (T–L) model. We deduced that the CsFAPI thin film had a slightly lower absorption coefficient than the FAPI, but a higher refractive index and dielectric constant than the FAPI. The peak photoluminescence (PL) emission of FAPI and CsFAPI thin film on glass substrates was observed around 803 nm and 799 nm, respectively, while on ITO substrates, both FAPI and CsFAPI thin film was quenched and red-shifted to 816 nm. The methylammonium free pure CsFAPI-based perovskite solar cell fabricated in p–i–n configuration, measured a competitive efficiency of 16.14%, characterized by a <em>J</em><small><sub>SC</sub></small> of 23.995 mA cm<small><sup>−2</sup></small>, <em>V</em><small><sub>OC</sub></small> of 912 mV, and FF of 73.74%.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 2512-2519"},"PeriodicalIF":3.2,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11369667/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142141910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Highly conductive flat grains of cesium lead bromide perovskites via additive engineering with methylammonium bromide† 通过溴化甲基铵添加工程获得高导电性扁平溴化铯铅包晶石晶粒
IF 3.2
Energy advances Pub Date : 2024-08-26 DOI: 10.1039/D4YA00487F
Chandra Shakher Pathak, Deepak Aloysius, Satyajit Gupta, Sabyasachi Mukhopadhyay and Eran Edri
{"title":"Highly conductive flat grains of cesium lead bromide perovskites via additive engineering with methylammonium bromide†","authors":"Chandra Shakher Pathak, Deepak Aloysius, Satyajit Gupta, Sabyasachi Mukhopadhyay and Eran Edri","doi":"10.1039/D4YA00487F","DOIUrl":"10.1039/D4YA00487F","url":null,"abstract":"<p >Perovskite solar cells made of inorganic cesium lead bromide (CsPbBr<small><sub>3</sub></small>) display unusually high open-circuit potentials. Yet, their photovoltaic efficiency is still lagging behind that of iodide-based halide perovskites. In this study, a multistep solution spin coating process is used to create a CsPbBr<small><sub>3</sub></small> film. The CsPbBr<small><sub>3</sub></small> perovskite film consists of flat and rounded grains, and the photocurrent of each grain type is imbalanced. Interestingly, a significant current increase in flat grains is observed when conducting atomic force microscopy (c-AFM) at the nanoscale after the addition of methyl ammonium bromide (MABr) as an additive. The addition of MABr results in good optoelectronic quality of perovskite films with highly conductive grains and enables better charge transport and hence improved power conversion efficiency.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 2543-2551"},"PeriodicalIF":3.2,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00487f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective kinetic control of interfacial charge transfer reactions in Si-composite anodes for Li-ion batteries† 锂离子电池硅复合材料阳极中界面电荷转移反应的选择性动力学控制†。
IF 3.2
Energy advances Pub Date : 2024-08-23 DOI: 10.1039/D4YA00418C
Emma A. Cave, Tyson A. Carr and Cody W. Schlenker
{"title":"Selective kinetic control of interfacial charge transfer reactions in Si-composite anodes for Li-ion batteries†","authors":"Emma A. Cave, Tyson A. Carr and Cody W. Schlenker","doi":"10.1039/D4YA00418C","DOIUrl":"https://doi.org/10.1039/D4YA00418C","url":null,"abstract":"<p >In this report, we demonstrate a strategy to selectively suppress reactions at unpassivated active material surfaces in silicon composite electrodes, mitigating the capacity-draining effects of continual electrolyte reduction in alloying-type anodes for lithium-ion batteries. Inspired by dipolar modification of electrodes for photovoltaic applications, we introduced conformationally-labile permanent dipoles at the electrochemical electrode interface to dynamically modulate charge transfer kinetics across the interface. Polyacrylic acid (PAA) binder modified with the dipole-bearing molecule 3-cyanopropyltriethoxysilane displays a 17% increase in capacity retention <em>versus</em> unmodified PAA binder. Differential capacity analysis shows a marked cathodic shift of ∼150 mV in overpotential in the pre-alloying voltage range following the initial solid electrolyte interphase (SEI) formation step. At the same time, we observe negligible shift in overpotential for reversible lithium-ion storage, consistent with selective modulation of irreversible reaction kinetics. Electrochemical impedance spectroscopy indicates that this modification results in a thinner SEI layer. Despite the improved performance, the charge transfer resistance of the half-cell is higher with the modification, suggesting some opportunity for improving the strategy. Time-resolved spectroelectrochemical analysis of desolvation kinetics in modified binders indicates that the modified binder has slower and less selective ion transport. We conclude that future iterations of this strategy which avoid disrupting the beneficial ionic transport properties of the binder would result in even greater performance enhancement. We propose that this may be accomplished by incorporating oligomeric dipolar modifiers, either in the binder or at the active material itself. Either way would increase the ratio of dipoles to PAA linking sites, thus avoiding the competing deleterious impacts on device performance.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 2186-2199"},"PeriodicalIF":3.2,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00418c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142174055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A cradle-to-gate life cycle assessment of green methanol production using direct air capture† 利用直接空气捕集技术进行绿色甲醇生产的 "从摇篮到终点 "生命周期评估†。
IF 3.2
Energy advances Pub Date : 2024-08-20 DOI: 10.1039/D4YA00316K
Nicholas Badger, Rahim Boylu, Valentine Ilojianya, Mustafa Erguvan and Shahriar Amini
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