Mingzhe Wang, Sisi Ling, Ziyan Zhang, Yejun Zhang, Hongchao Yang, Qiangbin Wang
Hydrophilic semiconductor quantum dots (QDs) with photoluminescence (PL) located in the second near-infrared window (NIR-II) have demonstrated great promise for in vivo bioimaging applications. However, their performance can be affected by the strong water absorption in this spectral region, which results in severely reduced NIR-II PL intensity. Herein, we used a polyethyleneglycol (PEG) modified with a hydrophobic alkyl chain (-C11H22-) to decorate non-toxic NIR-II Ag2S (Ag2S-C11-PEG) QDs. The incorporation of the alkyl chain minimizes the energy transfer process from QDs to water molecules. As a result, the Ag2S-C11-PEG QDs exhibit superior PL intensity with approximately three-fold enhancement to the Ag2S QDs coated by PEG without alkyl chain modification (Ag2S-PEG). In addition, the PEG skeleton ensures the stealth effect from macrophages resident in tissue and filtration organs (MPS system) and decent biocompatibility of the probe. Ultimately, the Ag2S-C11-PEG QDs have been demonstrated their potential as high-performance probes for in vivo bioimaging, exhibiting excellent brightness and metabolizable ability. This work showcases a valid strategy for advancing NIR-II QDs in high-performance bioimaging applications.
{"title":"Revealing the Energy Transfer between NIR-II PEGylated Quantum Dots and Water","authors":"Mingzhe Wang, Sisi Ling, Ziyan Zhang, Yejun Zhang, Hongchao Yang, Qiangbin Wang","doi":"10.1039/d4qi02869d","DOIUrl":"https://doi.org/10.1039/d4qi02869d","url":null,"abstract":"Hydrophilic semiconductor quantum dots (QDs) with photoluminescence (PL) located in the second near-infrared window (NIR-II) have demonstrated great promise for in vivo bioimaging applications. However, their performance can be affected by the strong water absorption in this spectral region, which results in severely reduced NIR-II PL intensity. Herein, we used a polyethyleneglycol (PEG) modified with a hydrophobic alkyl chain (-C11H22-) to decorate non-toxic NIR-II Ag2S (Ag2S-C11-PEG) QDs. The incorporation of the alkyl chain minimizes the energy transfer process from QDs to water molecules. As a result, the Ag2S-C11-PEG QDs exhibit superior PL intensity with approximately three-fold enhancement to the Ag2S QDs coated by PEG without alkyl chain modification (Ag2S-PEG). In addition, the PEG skeleton ensures the stealth effect from macrophages resident in tissue and filtration organs (MPS system) and decent biocompatibility of the probe. Ultimately, the Ag2S-C11-PEG QDs have been demonstrated their potential as high-performance probes for in vivo bioimaging, exhibiting excellent brightness and metabolizable ability. This work showcases a valid strategy for advancing NIR-II QDs in high-performance bioimaging applications.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"66 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486535","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junmou Du, Guocheng Li, Yuchen Tan, Xiangrui Duan, Tianchi Fan, Changhong Du, Anjian Zhou, Yu Wang
The pursuit of high-energy-density batteries has generated significant interest in lithium metal anodes due to their high specific capacity and low redox potential. However, challenges such as the formation of lithium dendrites and the subsequent generation of "dead lithium" during the plating/stripping processes seriously hinder their practical application. In this study, we present a novel composite lithium anode, Li/Li13Sn5, which is fabricated using a straightforward "roll and fold" technique that incorporates metallic lithium and tin powder. This method ensures a uniform distribution of Li13Sn5 particles within the lithium matrix, thereby enhancing the lithiophilicity of the composite electrode. The unique structural characteristics of the Li/Li13Sn5 anode lead to significantly improved. Compared to bare Li anode, the Li/Li13Sn5 anode exhibits a stable voltage response and reduced interfacial impedance in symmetric cells over 400 hours cycling. When paired with a high capacity sulfurized polyacrylonitrile (SPAN) cathode (5.6 mAh cm−2), the Li/Li13Sn5 cell displayed superior cycling stability, achieving 91.5% capacity retention over 100 cycles. This innovative approach, which leverages lithiophilic metal powders to build highly dispersed lithium alloy networks present a promising strategy for the advancement of lithium metal batteries. Our findings contribute to the development of composite lithium alloy anodes with high lithium alloy utilization, paving the way for next-generation lithium battery technologies.
{"title":"Tuning the Li-Sn alloy dispersity to improve the lithiophilicity of lithium metal anode towards stable lithium metal batteries","authors":"Junmou Du, Guocheng Li, Yuchen Tan, Xiangrui Duan, Tianchi Fan, Changhong Du, Anjian Zhou, Yu Wang","doi":"10.1039/d4qi02971b","DOIUrl":"https://doi.org/10.1039/d4qi02971b","url":null,"abstract":"The pursuit of high-energy-density batteries has generated significant interest in lithium metal anodes due to their high specific capacity and low redox potential. However, challenges such as the formation of lithium dendrites and the subsequent generation of \"dead lithium\" during the plating/stripping processes seriously hinder their practical application. In this study, we present a novel composite lithium anode, Li/Li13Sn5, which is fabricated using a straightforward \"roll and fold\" technique that incorporates metallic lithium and tin powder. This method ensures a uniform distribution of Li13Sn5 particles within the lithium matrix, thereby enhancing the lithiophilicity of the composite electrode. The unique structural characteristics of the Li/Li13Sn5 anode lead to significantly improved. Compared to bare Li anode, the Li/Li13Sn5 anode exhibits a stable voltage response and reduced interfacial impedance in symmetric cells over 400 hours cycling. When paired with a high capacity sulfurized polyacrylonitrile (SPAN) cathode (5.6 mAh cm−2), the Li/Li13Sn5 cell displayed superior cycling stability, achieving 91.5% capacity retention over 100 cycles. This innovative approach, which leverages lithiophilic metal powders to build highly dispersed lithium alloy networks present a promising strategy for the advancement of lithium metal batteries. Our findings contribute to the development of composite lithium alloy anodes with high lithium alloy utilization, paving the way for next-generation lithium battery technologies.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"27 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jing Su, Yin Fan, Xiao-Fang Duan, Jing-Yao Zhou, Lipeng Zhou, Chong-Bin Tian, Qing-Fu Sun
The synthesis of nonclassical polyhedra is at the forefront of supramolecular research for their unique anisotropic interior cavities. However, due to the difficulty in controlling the topology of Ln supramolecular systems, the preparation of nonclassical lanthanide organic polyhedral (LOPs) remains a challenge. Herein, we explore the ionic radius dependent self-assembly of LOPs using rectangular tetra-tropic ligand L. Due to the rectangular, other than square, geometry of the ligand panels, the assembly of it with lanthanide ions located in the middle of Ln series affords the irregular tetragonal antiprismatic Ln8L4 (Ln = Sm3+, Eu3+, Tb3+, Dy3+ and Ho3+) with two faces are unoccupied by ligands L. Interestingly, such tetragonal antiprism possesses an oblate internal cavity, which binds four THF molecules in the solid-state structure. With an increase in radius, the larger La3+ and Nd3+ ions, produces a distinct architecture, the sandwich square, Ln4L2. In contrast, the smaller Er3+ and Lu3+ ions give rise to a mixture of both Ln8L4 and Ln6L3. Once adding excess Ln3+ ions, the structure transformation from Ln8L4 to Ln6L3 occur. Structural comparisons of La4L2 and Sm8L4 reveal that the differences in architecture within these systems are governed by both the ionic radii of the lanthanides and the conformational flexibility of the ligands. Photophysical investigations disclose that the ligand L exhibits a sensitizing ability toward Sm3+, Tb3+ and Dy3+ ions, displaying their characteristic luminescence emission, with a new record-setting luminescent quantum yield of 92.74% being observed for Tb8L4. This work provides new insights to understand the effect of lanthanide size on the resulting assemblies and opens new avenues to develop nonclassical LOPs.
{"title":"Ionic Radius-Dependent Self-Assembly of Lanthanide Organic Polyhedra: Structural Diversities and Luminescent Properties","authors":"Jing Su, Yin Fan, Xiao-Fang Duan, Jing-Yao Zhou, Lipeng Zhou, Chong-Bin Tian, Qing-Fu Sun","doi":"10.1039/d5qi00265f","DOIUrl":"https://doi.org/10.1039/d5qi00265f","url":null,"abstract":"The synthesis of nonclassical polyhedra is at the forefront of supramolecular research for their unique anisotropic interior cavities. However, due to the difficulty in controlling the topology of Ln supramolecular systems, the preparation of nonclassical lanthanide organic polyhedral (LOPs) remains a challenge. Herein, we explore the ionic radius dependent self-assembly of LOPs using rectangular tetra-tropic ligand L. Due to the rectangular, other than square, geometry of the ligand panels, the assembly of it with lanthanide ions located in the middle of Ln series affords the irregular tetragonal antiprismatic Ln8L4 (Ln = Sm3+, Eu3+, Tb3+, Dy3+ and Ho3+) with two faces are unoccupied by ligands L. Interestingly, such tetragonal antiprism possesses an oblate internal cavity, which binds four THF molecules in the solid-state structure. With an increase in radius, the larger La3+ and Nd3+ ions, produces a distinct architecture, the sandwich square, Ln4L2. In contrast, the smaller Er3+ and Lu3+ ions give rise to a mixture of both Ln8L4 and Ln6L3. Once adding excess Ln3+ ions, the structure transformation from Ln8L4 to Ln6L3 occur. Structural comparisons of La4L2 and Sm8L4 reveal that the differences in architecture within these systems are governed by both the ionic radii of the lanthanides and the conformational flexibility of the ligands. Photophysical investigations disclose that the ligand L exhibits a sensitizing ability toward Sm3+, Tb3+ and Dy3+ ions, displaying their characteristic luminescence emission, with a new record-setting luminescent quantum yield of 92.74% being observed for Tb8L4. This work provides new insights to understand the effect of lanthanide size on the resulting assemblies and opens new avenues to develop nonclassical LOPs.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"208 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462511","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yijun Yu, Lei Liu, Puning Liu, Wannian Jiang, Zhonghua Zhang, Xiaosong Guo, Lin Zhang, Jun Zheng, Guicun Li
The solvation structure of electrolytes, particularly the distribution and composition of contact ion pairs (CIP) and solvent-separated ion pairs (SSIP), is a prominent focus in battery research, serving as a critical determinant for understanding and interpreting battery electrochemical behavior. In this work, a phosphate-enriched protective layer (ZAP) was fabricated on the Zn electrode via a simply displacement reaction to modify the adsorption properties of the Zn electrode, thereby influencing the composition of CIP and SSIP at the electrode-electrolyte interface. Experimental results revealed that the ZAP layer significantly reduced the overpotential for Zn deposition, particularly in low-concentration electrolytes and under high deposition currents. Through a series of characterizations and theoretical calculations, it was found that the ion concentrations at the electrode-electrolyte interface played a pivotal role in governing interfacial electrochemistry, surpassing the influence of the CIP-to-SSIP ratio in the bulk electrolyte. Moreover, the ZAP layer could effectively suppress side reactions and enhance cycling stability of batteries. This study introduces a simple and cost-effective approach for protecting Zn anodes and emphasizes the critical importance of interfacial ion concentrations in electrochemical analysis.
{"title":"Electrostatic Regulation of Zn2+ Ion Concentration on Electrodes and Its Impact on Electrochemical Performance","authors":"Yijun Yu, Lei Liu, Puning Liu, Wannian Jiang, Zhonghua Zhang, Xiaosong Guo, Lin Zhang, Jun Zheng, Guicun Li","doi":"10.1039/d5qi00097a","DOIUrl":"https://doi.org/10.1039/d5qi00097a","url":null,"abstract":"The solvation structure of electrolytes, particularly the distribution and composition of contact ion pairs (CIP) and solvent-separated ion pairs (SSIP), is a prominent focus in battery research, serving as a critical determinant for understanding and interpreting battery electrochemical behavior. In this work, a phosphate-enriched protective layer (ZAP) was fabricated on the Zn electrode via a simply displacement reaction to modify the adsorption properties of the Zn electrode, thereby influencing the composition of CIP and SSIP at the electrode-electrolyte interface. Experimental results revealed that the ZAP layer significantly reduced the overpotential for Zn deposition, particularly in low-concentration electrolytes and under high deposition currents. Through a series of characterizations and theoretical calculations, it was found that the ion concentrations at the electrode-electrolyte interface played a pivotal role in governing interfacial electrochemistry, surpassing the influence of the CIP-to-SSIP ratio in the bulk electrolyte. Moreover, the ZAP layer could effectively suppress side reactions and enhance cycling stability of batteries. This study introduces a simple and cost-effective approach for protecting Zn anodes and emphasizes the critical importance of interfacial ion concentrations in electrochemical analysis.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"15 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Metal halide perovskites, particularly lead-based compounds, manifest great potential in X-ray detection due to their exceptional light absorption coefficients, superior carrier mobility and cost-effective preparation methods. Despite recent significant advancements, the limitations of lead toxicity hinder their further application and encourage the exploration of environmentally friendly alternatives. Herein, a novel lead-free two-dimensional (2D) copper-based halide perovskite (2FEA)2CuCl4 (2FEA = 2,2-difluoroethylamine) single crystal is developed, which exhibits a highly sensitive response to X-ray illumination. Especially, an inch-sized single crystal of (2FEA)2CuCl4 with dimensions up to 30 × 28 × 0.5 mm3 is grown using a low-cost cooling crystallization method. Direct X-ray detectors fabricated from these single crystals demonstrated an exceptionally high sensitivity of 1106.44 μC Gyair-1 cm-2 at a 10 V bias, approximately 43 times higher than that of the conventional radiation-sensitive semiconductor α-Se (~25 μC Gyair-1 cm-2). Furthermore, (2FEA)2CuCl4 exhibits a stable baseline with the low dark current drift of 5.056 × 10-7 nA cm-1 s-1 V-1 and the low limit of detection of 130.1 nGyair s-1 at 10 V bias. These findings manifest the great potential of 2D copper-based hybrid perovskites for the next generation of highly sensitive X-ray detection, which sheds light on the rational crystal design of “green” radiation-sensitive hybrid perovskites.
{"title":"Inch-sized single crystal of radiation-sensitive copper-based hybrid perovskite for direct X-ray detection","authors":"Yicong Lv, Xiantan Lin, Fafa Wu, Zengshan Yue, Fen Zhang, Xiaoqi Li, Qingyin Wei, Kai Li, Qianxi Wang, Junhua Luo, Xitao Liu","doi":"10.1039/d5qi00263j","DOIUrl":"https://doi.org/10.1039/d5qi00263j","url":null,"abstract":"Metal halide perovskites, particularly lead-based compounds, manifest great potential in X-ray detection due to their exceptional light absorption coefficients, superior carrier mobility and cost-effective preparation methods. Despite recent significant advancements, the limitations of lead toxicity hinder their further application and encourage the exploration of environmentally friendly alternatives. Herein, a novel lead-free two-dimensional (2D) copper-based halide perovskite (2FEA)2CuCl4 (2FEA = 2,2-difluoroethylamine) single crystal is developed, which exhibits a highly sensitive response to X-ray illumination. Especially, an inch-sized single crystal of (2FEA)2CuCl4 with dimensions up to 30 × 28 × 0.5 mm3 is grown using a low-cost cooling crystallization method. Direct X-ray detectors fabricated from these single crystals demonstrated an exceptionally high sensitivity of 1106.44 μC Gyair-1 cm-2 at a 10 V bias, approximately 43 times higher than that of the conventional radiation-sensitive semiconductor α-Se (~25 μC Gyair-1 cm-2). Furthermore, (2FEA)2CuCl4 exhibits a stable baseline with the low dark current drift of 5.056 × 10-7 nA cm-1 s-1 V-1 and the low limit of detection of 130.1 nGyair s-1 at 10 V bias. These findings manifest the great potential of 2D copper-based hybrid perovskites for the next generation of highly sensitive X-ray detection, which sheds light on the rational crystal design of “green” radiation-sensitive hybrid perovskites.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"23 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451954","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrocatalysts with excellent selectivity and activity towards the target product are pivotal for N2 conversion and utilization. In this study, we systematically explored the nitrogen reduction reaction (NRR) catalytic performance of Mo-based single-atom catalysts (Mo-N4-SACs) through density functional theory (DFT) calculations. We changed the coordination environment of the single atom by placing the active center of the SACs at the edge or basal plane of N-doped graphene or changing the coordination atom of the active center. Among the four Mo-N4-SACs studied, Mo-ZZG demonstrated remarkable catalytic activity and selectivity for N2 reduction to NH3 with a limiting potential (UL) of −0.26 V. After considering the solvation effect, the potential determination step was N2 → N2H, and only the UL was increased, specifically to −0.42 V. In order to reduce the UL of the Mo-ZZ-edge (−0.85 V) for the NRR by replacing the N atom with an S or O atom, the UL of the O1-ZZ-edge was reduced to −0.58 V. This well illustrated that the catalytic activity could be effectively improved by rationally adjusting the position and coordination atoms of a single atom. This work provides valuable insights into the rational design and screening of efficient catalysts for N2 reduction.
{"title":"Regulating the coordination environment of single-atom catalysts anchored on nitrogen-doped graphene for efficient nitrogen reduction","authors":"Shuo Wang, Bo Zhu, Likai Yan","doi":"10.1039/d4qi03239j","DOIUrl":"https://doi.org/10.1039/d4qi03239j","url":null,"abstract":"Electrocatalysts with excellent selectivity and activity towards the target product are pivotal for N2 conversion and utilization. In this study, we systematically explored the nitrogen reduction reaction (NRR) catalytic performance of Mo-based single-atom catalysts (Mo-N<small><sub>4</sub></small>-SACs) through density functional theory (DFT) calculations. We changed the coordination environment of the single atom by placing the active center of the SACs at the edge or basal plane of N-doped graphene or changing the coordination atom of the active center. Among the four Mo-N<small><sub>4</sub></small>-SACs studied, Mo-ZZG demonstrated remarkable catalytic activity and selectivity for N<small><sub>2</sub></small> reduction to NH<small><sub>3</sub></small> with a limiting potential (<em>U</em><small><sub>L</sub></small>) of −0.26 V. After considering the solvation effect, the potential determination step was N<small><sub>2</sub></small> → N<small><sub>2</sub></small>H, and only the <em>U</em><small><sub>L</sub></small> was increased, specifically to −0.42 V. In order to reduce the <em>U</em><small><sub>L</sub></small> of the Mo-ZZ-edge (−0.85 V) for the NRR by replacing the N atom with an S or O atom, the <em>U</em><small><sub>L</sub></small> of the O1-ZZ-edge was reduced to −0.58 V. This well illustrated that the catalytic activity could be effectively improved by rationally adjusting the position and coordination atoms of a single atom. This work provides valuable insights into the rational design and screening of efficient catalysts for N<small><sub>2</sub></small> reduction.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"11 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rational design of highly active and durable oxygen reduction reaction (ORR) electrocatalysts to replace expensive platinum-based catalysts and significantly improve the electrocatalytic performance of rechargeable zinc-air batteries (ZABs) has become a key goal in the field of energy storage technology. Here, we modulate the coordination structure of single-atom Zn sites on N-doped graphene matrix by a rapid heating technology to enhance the ORR performance. In 0.1 M KOH solution, the half-wave potential (E1/2) of Zn-NG is 0.84 V, and it has good anti-Fenton reaction performance. The zinc-air battery assembled with Zn-NG as the cathode material has an open-circuit voltage (OCV) of up to 1.50 V, and exhibits a maximum power density of 158 mW cm-2 and excellent output stability for over 200 h. Theoretical calculations show that the Zn-N4G configuration exhibits lower ORR barrier than Zn-N2G and Zn-N3G structures. The rate-determining step on Zn-N2G and Zn-N3G is *O →* OH, and both show a reaction barrier significantly greater than 1.00 eV. In contrast, the rate-determining step on the Zn-N4G is *OH → * + H2O, and the energy barrier is only 0.68 eV, thus exhibiting better catalytic performance.
{"title":"Coordination modulation of single-atom Zn sites to boost oxygen reduction performance","authors":"Siying Zhang, Xue Bai, Tianmi Tang, Weidong Ruan, Jingqi Guan","doi":"10.1039/d4qi03126a","DOIUrl":"https://doi.org/10.1039/d4qi03126a","url":null,"abstract":"Rational design of highly active and durable oxygen reduction reaction (ORR) electrocatalysts to replace expensive platinum-based catalysts and significantly improve the electrocatalytic performance of rechargeable zinc-air batteries (ZABs) has become a key goal in the field of energy storage technology. Here, we modulate the coordination structure of single-atom Zn sites on N-doped graphene matrix by a rapid heating technology to enhance the ORR performance. In 0.1 M KOH solution, the half-wave potential (E1/2) of Zn-NG is 0.84 V, and it has good anti-Fenton reaction performance. The zinc-air battery assembled with Zn-NG as the cathode material has an open-circuit voltage (OCV) of up to 1.50 V, and exhibits a maximum power density of 158 mW cm-2 and excellent output stability for over 200 h. Theoretical calculations show that the Zn-N4G configuration exhibits lower ORR barrier than Zn-N2G and Zn-N3G structures. The rate-determining step on Zn-N2G and Zn-N3G is *O →* OH, and both show a reaction barrier significantly greater than 1.00 eV. In contrast, the rate-determining step on the Zn-N4G is *OH → * + H2O, and the energy barrier is only 0.68 eV, thus exhibiting better catalytic performance.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"82 10 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451952","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jeong Hyeon Kim, Juchan Hwang, Soon Joo Yoon, Jongmin Kim, Yoon Kyeung Lee, Kwangwook Park, Han Eol Lee
Correction for ‘Monolithic green-sensitive photodetectors enabled by a ZnSnN2/GaN nanorods/silicon double heterojunction’ by Jeong Hyeon Kim et al., Inorg. Chem. Front., 2025, https://doi.org/10.1039/d4qi02418d.
{"title":"Correction: Monolithic green-sensitive photodetectors enabled by a ZnSnN2/GaN nanorods/silicon double heterojunction","authors":"Jeong Hyeon Kim, Juchan Hwang, Soon Joo Yoon, Jongmin Kim, Yoon Kyeung Lee, Kwangwook Park, Han Eol Lee","doi":"10.1039/d5qi90017d","DOIUrl":"https://doi.org/10.1039/d5qi90017d","url":null,"abstract":"Correction for ‘Monolithic green-sensitive photodetectors enabled by a ZnSnN<small><sub>2</sub></small>/GaN nanorods/silicon double heterojunction’ by Jeong Hyeon Kim <em>et al.</em>, <em>Inorg. Chem. Front.</em>, 2025, https://doi.org/10.1039/d4qi02418d.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"88 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xinyi Wang, Xin Wen, Yuchen Yan, Jindong Chen, Guangsai Yang, Guang Peng, Ning Ye
Beryllium-based selenite has rarely been reported. Herein, the first two alkaline earth metal beryllium-based selenites, Ca3Be(SeO3)4 and SrBe(SeO3)2, have been synthesized by a mild hydrothermal method. Both of them feature unique [Be(SeO3)4]6- composite groups. Due to different connection forms of [Be(SeO3)4]6-, these two crystals exhibit significantly different optical anisotropy. From Ca3Be(SeO3)4 to SrBe(SeO3)2, the birefringence range from 0.005@546 nm to 0.058@546 nm. Theoretical calculations confirmed the dominant role of [SeO3]2- in the optical anisotropy of these two crystals. In addition, both of them exhibited large band gaps (5.40 and 5.28 eV) and high thermal stability (596 and 570 °C). This work demonstrates that the introduction of beryllium can effectively increase the band gap of selenite to over 5eV, and offers new ideas for the development of large bandgap selenite.
{"title":"From Ca3Be(SeO3)4 to SrBe(SeO3)2: Two Unprecedented Alkaline Earth Metal Beryllium Selenites with Large Band Gaps and Enhanced Birefringence","authors":"Xinyi Wang, Xin Wen, Yuchen Yan, Jindong Chen, Guangsai Yang, Guang Peng, Ning Ye","doi":"10.1039/d5qi00039d","DOIUrl":"https://doi.org/10.1039/d5qi00039d","url":null,"abstract":"Beryllium-based selenite has rarely been reported. Herein, the first two alkaline earth metal beryllium-based selenites, Ca3Be(SeO3)4 and SrBe(SeO3)2, have been synthesized by a mild hydrothermal method. Both of them feature unique [Be(SeO3)4]6- composite groups. Due to different connection forms of [Be(SeO3)4]6-, these two crystals exhibit significantly different optical anisotropy. From Ca3Be(SeO3)4 to SrBe(SeO3)2, the birefringence range from 0.005@546 nm to 0.058@546 nm. Theoretical calculations confirmed the dominant role of [SeO3]2- in the optical anisotropy of these two crystals. In addition, both of them exhibited large band gaps (5.40 and 5.28 eV) and high thermal stability (596 and 570 °C). This work demonstrates that the introduction of beryllium can effectively increase the band gap of selenite to over 5eV, and offers new ideas for the development of large bandgap selenite.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"5 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443713","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xueling Wei, Yang Jiao, Xiangyu Zou, Yuchen GUO, Wenhu Li, Taotao Ai
Hydrogen production through water splitting using transition metal-based phosphide electrocatalysts represents a highly promising and sustainable energy conversion strategy. In this study, phosphating and vacancies engineering through Ar plasma-assisted is achieved via a single-step process. Taking CoFePv with phosphorus vacancies (Pv) as bifunctional electrocatalysts, it effectively promotes both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), thereby significantly facilitating overall water splitting (OWS) in alkaline media. In OER and HER processes, the driving potentials needed to attain current density of 1 A cm-2 are only 382 and 367 mV, respectively. Furthermore, the CoFePv (+, −) OWS electrolyzer is capable of maintaining a current density of 2 A cm⁻² at 1.98 V under simulated industrial settings (6 M KOH, 80°C). It also demonstrates stable performance at a current density of 0.5 A cm⁻² for a duration of 100 hours. In-situ Raman spectroscopy observations show that Pv induce rapid catalyst phase reconstruction, thereby significantly enhancing the OER performance of CoFePv. Density functional theory (DFT) calculations demonstrate that phosphorus vacancies can modulate the electronic properties of Co-Fe-P, facilitate electron transfer, as well as optimize the adsorption and desorption of reaction intermediates.
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