Pub Date : 2025-02-12DOI: 10.1016/j.esci.2025.100378
Sixiao Liu , Jun Lu , Xu Yu , Huan Pang , Qiang Zhang , Ho Seok Park
A faster and more environmentally friendly nitrogen treatment solution is required to address the demand for nitrogen resources and the negative environmental impacts of human activities. Nitrogen electrochemistry thus has received major attention as an avenue for achieving sustainable nitrogen conversion. Here, we comprehensively review recent progress in the rational design of metal–organic framework nanoparticle composites (MOF–NP) for sustainable nitrogen electrochemistry. Three synthesis MOF–NPs strategies are addressed, focusing on the growth of MOFs on NPs, the loading of NPs onto/into MOFs, and the simultaneous formation of MOFs and NPs. We also discuss the unique features of MOF materials and their derivatives for use in nitrogen reduction, nitrate reduction, and ammonia oxidation reactions. The review closes by describing the prospects and challenges for MOF–NP-based electrocatalysts in nitrogen electrochemistry applications.
{"title":"Rational design of metal–organic framework-nanoparticle composite electrocatalysts for sustainable nitrogen electrochemistry","authors":"Sixiao Liu , Jun Lu , Xu Yu , Huan Pang , Qiang Zhang , Ho Seok Park","doi":"10.1016/j.esci.2025.100378","DOIUrl":"10.1016/j.esci.2025.100378","url":null,"abstract":"<div><div>A faster and more environmentally friendly nitrogen treatment solution is required to address the demand for nitrogen resources and the negative environmental impacts of human activities. Nitrogen electrochemistry thus has received major attention as an avenue for achieving sustainable nitrogen conversion. Here, we comprehensively review recent progress in the rational design of metal–organic framework nanoparticle composites (MOF–NP) for sustainable nitrogen electrochemistry. Three synthesis MOF–NPs strategies are addressed, focusing on the growth of MOFs on NPs, the loading of NPs onto/into MOFs, and the simultaneous formation of MOFs and NPs. We also discuss the unique features of MOF materials and their derivatives for use in nitrogen reduction, nitrate reduction, and ammonia oxidation reactions. The review closes by describing the prospects and challenges for MOF–NP-based electrocatalysts in nitrogen electrochemistry applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 6","pages":"Article 100378"},"PeriodicalIF":36.6,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145340504","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100325
Yu Tian , Cheng Lin , Xiangfeng Meng , Xiao Yu , Hailong Li , Rui Xiong
Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era. Different from traditional methods, this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning, which is used to rapidly and robustly predict polarization-free incremental capacity analysis (ICA) curves in minutes, and physical modeling, which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves. Only measured charging current and voltage signals are used. Results demonstrates that 11 points collected at any starting state-of-charge (SOC) in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error (RMSE) of 0.2774 Ah/V. Accordingly, battery status can be accurately elevated based on their degradation at both macro and electrode levels. Through transfer learning, such a method can also be adapted to different battery chemistries, indicating the enticing potential for wide applications.
{"title":"Accelerated commercial battery electrode-level degradation diagnosis via only 11-point charging segments","authors":"Yu Tian , Cheng Lin , Xiangfeng Meng , Xiao Yu , Hailong Li , Rui Xiong","doi":"10.1016/j.esci.2024.100325","DOIUrl":"10.1016/j.esci.2024.100325","url":null,"abstract":"<div><div>Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era. Different from traditional methods, this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning, which is used to rapidly and robustly predict polarization-free incremental capacity analysis (ICA) curves in minutes, and physical modeling, which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves. Only measured charging current and voltage signals are used. Results demonstrates that 11 points collected at any starting state-of-charge (SOC) in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error (RMSE) of 0.2774 Ah/V. Accordingly, battery status can be accurately elevated based on their degradation at both macro and electrode levels. Through transfer learning, such a method can also be adapted to different battery chemistries, indicating the enticing potential for wide applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100325"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145136","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100310
Tiansheng Bai , Jiaxian Wang , Hongqiang Zhang , Fengjun Ji , Wei Song , Shenyi Xiao , Dandan Gao , Jingyu Lu , Lijie Ci , Deping Li
The Li–O2 battery (LOB) has attracted growing interest, including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity. However, a series of challenges have seriously hindered LOB development, such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions (ORR/OER) at the cathode, the formation of lithium dendrites, and undesirable corrosion at the lithium metal anode. Herein, we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode. The resultant LOB delivers a superior discharge capacity (> 16,000 mAh g−1), excellent long-term cycling stability (> 200 cycles), and enhanced high rate capability (> 300 cycles @ 500 mA g−1). The working mechanisms of these atomic Ni catalysts are revealed through carefully designed in situ experiments and theoretical calculations. This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.
由于其极高的理论比容量，锂氧电池（LOB）在下一代储能系统中具有巨大的潜力，因此引起了人们越来越多的兴趣。然而，一系列挑战严重阻碍了LOB的发展，例如阴极氧还原和析氧反应（ORR/OER）动力学缓慢，锂枝晶的形成以及锂金属阳极的不良腐蚀。在此，我们提出了一种基于超低负载镍原子催化剂的策略，以同时提高阴极的ORR/OER，同时稳定锂金属阳极。由此产生的LOB提供了卓越的放电能力(>；16,000 mA h g−1)，优异的长期循环稳定性(>；200个周期)，以及增强的高速率能力(>；300个周期@ 500 mA g−1)。通过精心设计的原位实验和理论计算，揭示了这些Ni原子催化剂的工作机理。这项工作为设计可用于实际应用的高性能lob提供了一种新的研究范式。
{"title":"Atomic Ni-catalyzed cathode and stabilized Li metal anode for high-performance Li–O2 batteries","authors":"Tiansheng Bai , Jiaxian Wang , Hongqiang Zhang , Fengjun Ji , Wei Song , Shenyi Xiao , Dandan Gao , Jingyu Lu , Lijie Ci , Deping Li","doi":"10.1016/j.esci.2024.100310","DOIUrl":"10.1016/j.esci.2024.100310","url":null,"abstract":"<div><div>The Li–O<sub>2</sub> battery (LOB) has attracted growing interest, including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity. However, a series of challenges have seriously hindered LOB development, such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions (ORR/OER) at the cathode, the formation of lithium dendrites, and undesirable corrosion at the lithium metal anode. Herein, we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode. The resultant LOB delivers a superior discharge capacity (> 16,000 mAh g<sup>−1</sup>), excellent long-term cycling stability (> 200 cycles), and enhanced high rate capability (> 300 cycles @ 500 mA g<sup>−1</sup>). The working mechanisms of these atomic Ni catalysts are revealed through carefully designed <em>in situ</em> experiments and theoretical calculations. This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100310"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143144268","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100278
Wen Yu , Nanping Deng , Yang Feng , Xiaofan Feng , Hengying Xiang , Lu Gao , Bowen Cheng , Weimin Kang , Kai Zhang
Solid-state lithium battery (SSLB) is considered as one of the promising candidates for next-generation power batteries due to high safety, unprecedented energy density and favorable adaptability to high pression and temperature. However, the system of solid electrolyte (SE), as one of the most important components in SSLB, is usually plagued by clumsy ionic transport, leading to poor rate performance of the SSLBs. Herein, a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Li+ at multi-scale, including microscopic, mesoscopic and macroscopic scales. The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth. Furthermore, some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically, involving the modulation of microscopic homogeneous structure, mesoscopic heterogeneous structure and macroscopic structures, etc. The proposed generalized rules for SEs are expected to construct a close link from mechanism−structure−characterization to high performances for SSLBs.
{"title":"Understanding multi-scale ion-transport in solid-state lithium batteries","authors":"Wen Yu , Nanping Deng , Yang Feng , Xiaofan Feng , Hengying Xiang , Lu Gao , Bowen Cheng , Weimin Kang , Kai Zhang","doi":"10.1016/j.esci.2024.100278","DOIUrl":"10.1016/j.esci.2024.100278","url":null,"abstract":"<div><div>Solid-state lithium battery (SSLB) is considered as one of the promising candidates for next-generation power batteries due to high safety, unprecedented energy density and favorable adaptability to high pression and temperature. However, the system of solid electrolyte (SE), as one of the most important components in SSLB, is usually plagued by clumsy ionic transport, leading to poor rate performance of the SSLBs. Herein, a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Li<sup>+</sup> at multi-scale, including microscopic, mesoscopic and macroscopic scales. The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth. Furthermore, some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically, involving the modulation of microscopic homogeneous structure, mesoscopic heterogeneous structure and macroscopic structures, etc. The proposed generalized rules for SEs are expected to construct a close link from mechanism−structure−characterization to high performances for SSLBs.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100278"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141053573","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100281
Hongyang Chen , Junxiong Wu , Manxian Li , Jingyue Zhao , Zulin Li , Manxi Wang , Xuan Li , Chuanping Li , Xiaochuan Chen , Xiaoyan Li , Yiu-Wing Mai , Yuming Chen
The growth of dendrites in Li/Na metal batteries is a multifaceted process that is controlled by several factors such as electric field, ion transportation, temperature, and pressure. Rational design of battery components has become a viable approach to address this challenge. Among the various design strategies, heterogeneous structures have been demonstrated to be effective in mitigating uneven metal deposition by reducing the local current density and regulating the deposition sites. In this review, we discuss comprehensively the underlying principles and factors that influence dendrite growth, as well as the synthesis approaches for heterogeneous structures. Furthermore, we provide an overview of the diverse applications of heterogeneous structures in battery components. Finally, we highlight existing challenges and future directions for the use of heterogeneous structures in regulating metal deposition.
{"title":"Heterogeneous structure design for stable Li/Na metal batteries: Progress and prospects","authors":"Hongyang Chen , Junxiong Wu , Manxian Li , Jingyue Zhao , Zulin Li , Manxi Wang , Xuan Li , Chuanping Li , Xiaochuan Chen , Xiaoyan Li , Yiu-Wing Mai , Yuming Chen","doi":"10.1016/j.esci.2024.100281","DOIUrl":"10.1016/j.esci.2024.100281","url":null,"abstract":"<div><div>The growth of dendrites in Li/Na metal batteries is a multifaceted process that is controlled by several factors such as electric field, ion transportation, temperature, and pressure. Rational design of battery components has become a viable approach to address this challenge. Among the various design strategies, heterogeneous structures have been demonstrated to be effective in mitigating uneven metal deposition by reducing the local current density and regulating the deposition sites. In this review, we discuss comprehensively the underlying principles and factors that influence dendrite growth, as well as the synthesis approaches for heterogeneous structures. Furthermore, we provide an overview of the diverse applications of heterogeneous structures in battery components. Finally, we highlight existing challenges and future directions for the use of heterogeneous structures in regulating metal deposition.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100281"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141141564","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100279
Dandan Wang , Yusheng Li , Yongge Yang , Chao Ding , Yuyao Wei , Dong Liu , Hua Li , Huan Bi , Shikai Chen , Sujun Ji , Boyu Zhang , Yao Guo , Huiyun Wei , Hongshi Li , Shuzi Hayase , Qing Shen
Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorder and its impact on optical properties is crucial for overcoming this limitation. Here, using temperature-dependent static and transient absorption spectroscopy, we meticulously distinguish the contributions of static disorder (including defects, impurities, etc.) and dynamic disorder (carrier–phonon interactions). We reveal how these disorders shape band-tail structure and ultimately influence inter-band carrier recombination behaviors. Surprisingly, we find that static and dynamic disorder primarily control band-tail defect states and bandgap renormalization, respectively, which together modulate fast carrier trapping and slow band-band recombination rates. Furthermore, we link these disorders to the tin-induced symmetry-lowering distortions in tin-lead alloyed PNCs. These findings illuminate critical design principles for highly luminescent, low-toxicity tin-lead PNCs, accelerating their adoption in optoelectronic applications.
{"title":"Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals","authors":"Dandan Wang , Yusheng Li , Yongge Yang , Chao Ding , Yuyao Wei , Dong Liu , Hua Li , Huan Bi , Shikai Chen , Sujun Ji , Boyu Zhang , Yao Guo , Huiyun Wei , Hongshi Li , Shuzi Hayase , Qing Shen","doi":"10.1016/j.esci.2024.100279","DOIUrl":"10.1016/j.esci.2024.100279","url":null,"abstract":"<div><div>Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorder and its impact on optical properties is crucial for overcoming this limitation. Here, using temperature-dependent static and transient absorption spectroscopy, we meticulously distinguish the contributions of static disorder (including defects, impurities, etc.) and dynamic disorder (carrier–phonon interactions). We reveal how these disorders shape band-tail structure and ultimately influence inter-band carrier recombination behaviors. Surprisingly, we find that static and dynamic disorder primarily control band-tail defect states and bandgap renormalization, respectively, which together modulate fast carrier trapping and slow band-band recombination rates. Furthermore, we link these disorders to the tin-induced symmetry-lowering distortions in tin-lead alloyed PNCs. These findings illuminate critical design principles for highly luminescent, low-toxicity tin-lead PNCs, accelerating their adoption in optoelectronic applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100279"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141027486","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100307
Cong-Hui Li , Cheng-Zong Yuan , Xiaolei Huang , Hongrui Zhao , Fuling Wu , Lei Xin , Xiaomeng Zhang , Shufeng Ye , Yunfa Chen
Stabilizing the highly active RuO2 electrocatalyst for the oxygen evolution reaction (OER) is critical for the application of proton exchange membrane water electrolysis, but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments. Herein, we describe constructing Ru-O-La asymmetric configurations into RuO2 via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers. Specifically, the as-prepared optimal La0.1Ru0.9O2 shows a low overpotential of 188 mV at 10 mA cm−2, a high mass activity of 251 A at 1.6 V vs. reversible hydrogen electrode (RHE), and a long-lasting durability of 63 h, far superior to the 8 h achieved by standard RuO2. Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO2. More importantly, electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru, thus preventing the over-oxidation of Ru. In addition, electron redistribution tunes the Ru 4d band center’s energy level, which optimizes the adsorption and desorption of oxygen intermediates. This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO2-based acidic OER electrocatalysts.
稳定出氧反应（OER）的高活性RuO2电催化剂对于质子交换膜电解的应用至关重要，但由于Ru在恶劣的氧化环境中不可避免的过度氧化，这仍然具有挑战性。在这里，我们描述了通过简单的溶胶-凝胶方法构建Ru- o - la不对称构型到RuO2中，以调整电子再分配，从而消除Ru中心的过度氧化。具体而言，制备的最佳La0.1Ru0.9O2在10 mA cm−2下的过电位为188 mV，与可逆氢电极（RHE）相比，在1.6 V下的质量活性高达251 a gRu−1，持久寿命为63 h，远远优于标准RuO2的8 h。实验和密度泛函理论计算共同表明，Ru-O-La的不对称构型可以引发RuO2中的电子重分布。更重要的是，电子通过Ru- o -La结构从La转移到Ru，可以增加Ru周围的电子密度，从而防止Ru的过度氧化。此外，电子重分配调节了Ru 4d带中心的能级，从而优化了氧中间体的吸附和解吸。本研究提供了一种有效的策略来调节电子结构，以协同提高基于ruo2的酸性OER电催化剂的活性和稳定性。
{"title":"Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution","authors":"Cong-Hui Li , Cheng-Zong Yuan , Xiaolei Huang , Hongrui Zhao , Fuling Wu , Lei Xin , Xiaomeng Zhang , Shufeng Ye , Yunfa Chen","doi":"10.1016/j.esci.2024.100307","DOIUrl":"10.1016/j.esci.2024.100307","url":null,"abstract":"<div><div>Stabilizing the highly active RuO<sub>2</sub> electrocatalyst for the oxygen evolution reaction (OER) is critical for the application of proton exchange membrane water electrolysis, but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments. Herein, we describe constructing Ru-O-La asymmetric configurations into RuO<sub>2</sub> via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers. Specifically, the as-prepared optimal La<sub>0.1</sub>Ru<sub>0.9</sub>O<sub>2</sub> shows a low overpotential of 188 mV at 10 mA cm<sup>−2</sup>, a high mass activity of 251 A <span><math><mrow><msup><msub><mi>g</mi><mtext>Ru</mtext></msub><mrow><mo>−</mo><mn>1</mn></mrow></msup></mrow></math></span> at 1.6 V vs. reversible hydrogen electrode (RHE), and a long-lasting durability of 63 h, far superior to the 8 h achieved by standard RuO<sub>2</sub>. Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO<sub>2</sub>. More importantly, electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru, thus preventing the over-oxidation of Ru. In addition, electron redistribution tunes the Ru 4d band center’s energy level, which optimizes the adsorption and desorption of oxygen intermediates. This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO<sub>2</sub>-based acidic OER electrocatalysts.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100307"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145137","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100242
Bing He , Yu Cao , Kaijie Lin , Mingjie Wu , Yunhai Zhu , Xun Cui , Liang Hu , Yingkui Yang , Xueqin Liu
Bismuth vanadate (BiVO4) is a promising photoanode material for photoelectrochemical (PEC) water oxidation. However, its performance is greatly hindered by poor bulk and interfacial charge transfer. Herein, to address this issue, iron doped vanadyl phosphate (Fe:VOPO4) was grafted on molybdenum doped BiVO4 (Mo:BiVO4) for significantly enhancing charge transfer and oxygen evolution kinetics simultaneously. Consequently, the resultant Fe:VOPO4/Mo:BVO4 photoanode exhibits a remarkable photocurrent density of 6.59 mA cm−2 at 1.23 V versus the reversible hydrogen electrode (VRHE) under AM 1.5G illumination, over approximately 5.5 times as high as that of pristine BiVO4. Systematic studies have demonstrated that the hopping activation energy of small polarons is significantly reduced due to the Mo doping, resulting in accelerated bulk charge transfer. More importantly, the deposition of Fe:VOPO4 promotes the interfacial charge transfer between Mo:BiVO4 and Fe:VOPO4 via the construction of V–O–V and P–O bonds, in addition to facilitating water splitting kinetics. This work provides a general strategy for optimizing charge transfer process, especially at the interface between photoanodes and cocatalysts.
钒酸铋（BiVO4）是一种很有前途的光电化学（PEC）水氧化光阳极材料。然而，其性能却因体积和界面电荷转移能力差而大受影响。为了解决这一问题，本文将掺杂铁的磷酸钒（Fe:VOPO4）接枝到掺杂钼的 BiVO4（Mo:BiVO4）上，以同时显著增强电荷转移和氧进化动力学。因此，在 AM 1.5G 光照下，Fe:VOPO4/Mo:BVO4 光阳极在 1.23 V 电压下与可逆氢电极 (VRHE) 相比显示出 6.59 mA cm-2 的显著光电流密度，是原始 BiVO4 光阳极的 5.5 倍以上。系统研究表明，由于掺杂了钼，小极子的跳跃活化能显著降低，从而加速了体电荷转移。更重要的是，Fe:VOPO4 的沉积通过构建 V-O-V 和 P-O 键，促进了 Mo:BiVO4 和 Fe:VOPO4 之间的界面电荷转移，此外还有利于水分离动力学。这项工作为优化电荷转移过程，尤其是光阳极与助催化剂之间的界面电荷转移过程提供了一种通用策略。
{"title":"Enhanced bulk and interfacial charge transfer in Fe:VOPO4 modified Mo:BiVO4 photoanodes for photoelectrochemical water splitting","authors":"Bing He , Yu Cao , Kaijie Lin , Mingjie Wu , Yunhai Zhu , Xun Cui , Liang Hu , Yingkui Yang , Xueqin Liu","doi":"10.1016/j.esci.2024.100242","DOIUrl":"10.1016/j.esci.2024.100242","url":null,"abstract":"<div><div>Bismuth vanadate (BiVO<sub>4</sub>) is a promising photoanode material for photoelectrochemical (PEC) water oxidation. However, its performance is greatly hindered by poor bulk and interfacial charge transfer. Herein, to address this issue, iron doped vanadyl phosphate (Fe:VOPO<sub>4</sub>) was grafted on molybdenum doped BiVO<sub>4</sub> (Mo:BiVO<sub>4</sub>) for significantly enhancing charge transfer and oxygen evolution kinetics simultaneously. Consequently, the resultant Fe:VOPO<sub>4</sub>/Mo:BVO<sub>4</sub> photoanode exhibits a remarkable photocurrent density of 6.59 mA cm<sup>−2</sup> at 1.23 V versus the reversible hydrogen electrode (V<sub>RHE</sub>) under AM 1.5G illumination, over approximately 5.5 times as high as that of pristine BiVO<sub>4</sub>. Systematic studies have demonstrated that the hopping activation energy of small polarons is significantly reduced due to the Mo doping, resulting in accelerated bulk charge transfer. More importantly, the deposition of Fe:VOPO<sub>4</sub> promotes the interfacial charge transfer between Mo:BiVO<sub>4</sub> and Fe:VOPO<sub>4</sub> via the construction of V–O–V and P–O bonds, in addition to facilitating water splitting kinetics. This work provides a general strategy for optimizing charge transfer process, especially at the interface between photoanodes and cocatalysts.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100242"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139506761","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100264
Liu Lin , Peiyuan Su , Yiting Han , Yunming Xu , Qiao Ni , Xinyue Zhang , Peixun Xiong , Zemin Sun , Genban Sun , Xuebo Chen
Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy. Electrocatalytic reactions occur at the interface of catalysts, where the physicochemical properties of the catalyst surface play a dominant role. In particular, the electron spin behavior on the catalyst surface has a decisive impact on the catalytic reaction process. This review initially introduces the definition of electron spin and methods for spin manipulation. Furthermore, we summarize the advanced characterization methods of electron spin. Then, we review the latest research advancements on the spin effect in the oxygen reduction reaction, oxygen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. The catalytic mechanisms of spin manipulation in these four reactions are thoroughly discussed. Finally, we propose key directions for the future development of spin effects in the field of electrocatalysis. This review contributes to a deeper understanding of the micromechanisms in electrocatalytic reactions.
{"title":"Advances in regulating the electron spin effect toward electrocatalysis applications","authors":"Liu Lin , Peiyuan Su , Yiting Han , Yunming Xu , Qiao Ni , Xinyue Zhang , Peixun Xiong , Zemin Sun , Genban Sun , Xuebo Chen","doi":"10.1016/j.esci.2024.100264","DOIUrl":"10.1016/j.esci.2024.100264","url":null,"abstract":"<div><div>Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy. Electrocatalytic reactions occur at the interface of catalysts, where the physicochemical properties of the catalyst surface play a dominant role. In particular, the electron spin behavior on the catalyst surface has a decisive impact on the catalytic reaction process. This review initially introduces the definition of electron spin and methods for spin manipulation. Furthermore, we summarize the advanced characterization methods of electron spin. Then, we review the latest research advancements on the spin effect in the oxygen reduction reaction, oxygen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. The catalytic mechanisms of spin manipulation in these four reactions are thoroughly discussed. Finally, we propose key directions for the future development of spin effects in the field of electrocatalysis. This review contributes to a deeper understanding of the micromechanisms in electrocatalytic reactions.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100264"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140270528","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}
Pub Date : 2025-01-01DOI: 10.1016/j.esci.2024.100267
Jianwen Liu , Guodong Fu , Yuanfeng Liao , Wangji Zhang , Xiuan Xi , Fengzhan Si , Lei Wang , Jiujun Zhang , Xian-Zhu Fu , Jing-Li Luo
The electrochemical conversion of small organic molecules to value-added chemicals and hydrogen/electricity without CO2 emissions integrates efficient energy conversions (hydrogen energy or electricity) and value-added chemical productions in one reaction system, which is essentially competitive in the carbon-neutral era. However, the activity, stability, and cost-effectiveness of electrocatalysts, as well as the safety, durability, and scalability of devices, are still challenging for their industrial applications. In addition, a lack of knowledge about relevant and detailed mechanisms restricts the further development of electrocatalysts and devices. A timely review of the electrocatalysts, devices, and mechanisms is essential to shed lights on the correct direction towards further development. In this review, the advances in the design of electrocatalysts, fabrication of devices, and understanding of reaction mechanisms are comprehensively summarized and analyzed. The major challenges are also discussed as well as the potential approaches to overcoming them. The insights for further development are provided to offer a sustainable and environmentally friendly approach to cogeneration of energy and chemicals production.
{"title":"Electrochemical conversion of small organic molecules to value-added chemicals and hydrogen/electricity without CO2 emission: Electrocatalysts, devices and mechanisms","authors":"Jianwen Liu , Guodong Fu , Yuanfeng Liao , Wangji Zhang , Xiuan Xi , Fengzhan Si , Lei Wang , Jiujun Zhang , Xian-Zhu Fu , Jing-Li Luo","doi":"10.1016/j.esci.2024.100267","DOIUrl":"10.1016/j.esci.2024.100267","url":null,"abstract":"<div><div>The electrochemical conversion of small organic molecules to value-added chemicals and hydrogen/electricity without CO<sub>2</sub> emissions integrates efficient energy conversions (hydrogen energy or electricity) and value-added chemical productions in one reaction system, which is essentially competitive in the carbon-neutral era. However, the activity, stability, and cost-effectiveness of electrocatalysts, as well as the safety, durability, and scalability of devices, are still challenging for their industrial applications. In addition, a lack of knowledge about relevant and detailed mechanisms restricts the further development of electrocatalysts and devices. A timely review of the electrocatalysts, devices, and mechanisms is essential to shed lights on the correct direction towards further development. In this review, the advances in the design of electrocatalysts, fabrication of devices, and understanding of reaction mechanisms are comprehensively summarized and analyzed. The major challenges are also discussed as well as the potential approaches to overcoming them. The insights for further development are provided to offer a sustainable and environmentally friendly approach to cogeneration of energy and chemicals production.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 1","pages":"Article 100267"},"PeriodicalIF":42.9,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140400771","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}
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