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Supporting Information: Fig. S30: There were inadvertent misplacements of images: “Dark” (Light 0 min) group was misplaced as “No PTZSPy + 15 min Light” (control) group; “No PTZSPy + 15 min Light” (control) group was misplaced as “Dark” (Light 0 min) group. The corrected images, obtained from the original data, should appear as shown below. These changes do not affect the interpretation of data or the conclusion of the study.[Formula presented]

The combination of cancer cell-activated fluorescence and the advantages of both type I and type II photodynamic therapy (PDT) capabilities to achieve a synergistic therapeutic effect in a complex tumor environment is highly desirable. Herein, we report an approach by means of tumor intracellular hypochlorite (ClO−) to turn on fluorescence integrated with type I and II ROS generation for imaging-guided PDT. The resultant PTZSPy functions as a type II photosensitizer with mitochondria-targeting capability. In the presence of ClO−, PTZSPy is transformed into its oxidized counterpart SPTZSPy, turns on an orange-red fluorescence and triggers the type I ROS generation ability. Biological studies revealed that PTZSPy can accurately distinguishes tumor cells from normal cells, dynamically monitors the cell ablation process and be utilized for theranostics in MCF-7 tumor-bearing nude mice in vivo. This work provides an innovative strategy exploiting the highly abundant ClO− in tumor cells for the type I and II ROS two-pronged and imaging-guided PDT. © 2023

Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li1.2Mn0.6Ni0.2O2 was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P5+ doping increased the distance between the (003) crystal planes from ∼0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.

Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li1.2Mn0.6Ni0.2O2 was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P5+ doping increased the distance between the (003) crystal planes from ∼0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.

Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li1.2Mn0.6Ni0.2O2 was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P5+ doping increased the distance between the (003) crystal planes from ∼0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.

Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li1.2Mn0.6Ni0.2O2 was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P5+ doping increased the distance between the (003) crystal planes from ∼0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.

Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li1.2Mn0.6Ni0.2O2 was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P5+ doping increased the distance between the (003) crystal planes from ∼0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.

One of the key challenges toward high-power Li-ion batteries is to develop cheap, easy-to-prepare materials that combine high volumetric and gravimetric energy density with high power densities and a long cycle life. This requires electrode materials with large tap densities, which generally compromises the charge transport and hence the power density. Here densely packed Li4Ti5O12 (LTO) submicrospheres are prepared via a simple and easily up-scalable self-assembly process, resulting in very high tap densities (1.2 g.cm(-2)) and displaying exceptionally stable long-term high rate cyclic performance. The specific capacities at a (dis) charge rate of 10 and 20 C reach 148.6 and 130.1 mAh g(-1), respectively. Moreover, the capacity retention ratio is 97.3% after 500 cycles at 10 C in a half cell, and no obvious capacity reduction is found even after 8000 cycles at 30 C in a full LiFePO4/LTO battery. The excellent performance is explained by the abundant presence of grain boundaries between the nanocrystallites in the submicron spheres creating a 3D interconnected network, which allows very fast Li-ion and electron transport as indicated by the unusually large Li-ion diffusion coefficients and electronic conductivity at (6.2 x 10(-12) cm(2) s(-1) at 52% SOC and 3.8 X 10(-6) S cm(-1), respectively). This work demonstrates that, unlike in porous and nanosheet LTO structures with a high carbon content, exceptionally high rate charge transport can be combined with a large tap density and hence a large volumetric energy density, with the additional advantage of a much longer cycle life. More generally, the present results provide a promising strategy toward electrode materials combining high rate performances with high volumetric energy densities and long-term cyclic stability as required for the application in electric vehicles and tools.

One of the key challenges toward high-power Li-ion batteries is to develop cheap, easy-to-prepare materials that combine high volumetric and gravimetric energy density with high power densities and a long cycle life. This requires electrode materials with large tap densities, which generally compromises the charge transport and hence the power density. Here densely packed Li4Ti5O12 (LTO) submicrospheres are prepared via a simple and easily up-scalable self-assembly process, resulting in very high tap densities (1.2 g.cm(-2)) and displaying exceptionally stable long-term high rate cyclic performance. The specific capacities at a (dis) charge rate of 10 and 20 C reach 148.6 and 130.1 mAh g(-1), respectively. Moreover, the capacity retention ratio is 97.3% after 500 cycles at 10 C in a half cell, and no obvious capacity reduction is found even after 8000 cycles at 30 C in a full LiFePO4/LTO battery. The excellent performance is explained by the abundant presence of grain boundaries between the nanocrystallites in the submicron spheres creating a 3D interconnected network, which allows very fast Li-ion and electron transport as indicated by the unusually large Li-ion diffusion coefficients and electronic conductivity at (6.2 x 10(-12) cm(2) s(-1) at 52% SOC and 3.8 X 10(-6) S cm(-1), respectively). This work demonstrates that, unlike in porous and nanosheet LTO structures with a high carbon content, exceptionally high rate charge transport can be combined with a large tap density and hence a large volumetric energy density, with the additional advantage of a much longer cycle life. More generally, the present results provide a promising strategy toward electrode materials combining high rate performances with high volumetric energy densities and long-term cyclic stability as required for the application in electric vehicles and tools.

One of the key challenges toward high-power Li-ion batteries is to develop cheap, easy-to-prepare materials that combine high volumetric and gravimetric energy density with high power densities and a long cycle life. This requires electrode materials with large tap densities, which generally compromises the charge transport and hence the power density. Here densely packed Li4Ti5O12 (LTO) submicrospheres are prepared via a simple and easily up-scalable self-assembly process, resulting in very high tap densities (1.2 g.cm(-2)) and displaying exceptionally stable long-term high rate cyclic performance. The specific capacities at a (dis) charge rate of 10 and 20 C reach 148.6 and 130.1 mAh g(-1), respectively. Moreover, the capacity retention ratio is 97.3% after 500 cycles at 10 C in a half cell, and no obvious capacity reduction is found even after 8000 cycles at 30 C in a full LiFePO4/LTO battery. The excellent performance is explained by the abundant presence of grain boundaries between the nanocrystallites in the submicron spheres creating a 3D interconnected network, which allows very fast Li-ion and electron transport as indicated by the unusually large Li-ion diffusion coefficients and electronic conductivity at (6.2 x 10(-12) cm(2) s(-1) at 52% SOC and 3.8 X 10(-6) S cm(-1), respectively). This work demonstrates that, unlike in porous and nanosheet LTO structures with a high carbon content, exceptionally high rate charge transport can be combined with a large tap density and hence a large volumetric energy density, with the additional advantage of a much longer cycle life. More generally, the present results provide a promising strategy toward electrode materials combining high rate performances with high volumetric energy densities and long-term cyclic stability as required for the application in electric vehicles and tools.