Controlled C-N configurations,i.e.,pyrrolic-N,pyridinic-N,and graphitic-N,are promising strategies to tailor the carbon dots’(CDs)optical properties into the first near infrared(NIR)window(650-900 nm),a responsive ra...Controlled C-N configurations,i.e.,pyrrolic-N,pyridinic-N,and graphitic-N,are promising strategies to tailor the carbon dots’(CDs)optical properties into the first near infrared(NIR)window(650-900 nm),a responsive range for biomedical application.However,a deep understanding of the role of the C-N configuration in the CDs’properties is still challenging and thoughtprovoking owing to their complex structure.Here,an underlying pyrrolic-N concentration and position effect on the pyrrolic-N-rich CDs’absorption was comprehensively elucidated based on the integrated experimental and computational studies.The assynthesized pyrrolic-N-rich CDs exhibit a first NIR window absorption centered at 650 nm with high photothermal conversion.Pyrrolic-N concentrations from 1.4%to 11.3%and positions(edge and mid-site)were systematically investigated.A mid-site pyrrolic-N was subsequently generated after the pyrrolic-N concentration more than 10%.Edge-site pyrrolic-N induces a frontier orbital hybridization,reducing bandgap energy,while mid-site pyrrolic-N plays a critical role in inducing a first NIR window absorption owing to their high charge transfer.Also,pyrrolic-N-rich CDs inherit a bowl-like topological feature,elevating the CDs’layer thickness as much as 0.71 nm.This study shed light on the design and optimization of pyrrolic-N on CDs for the first NIR window responsive materials in any biomedical application.展开更多
Equity and efficiency are two important factors guiding the mitigation of anthropogenic emissions to achieve the Paris climate goals.Previous studies have proposed a range of allocations of global carbon budgets,but f...Equity and efficiency are two important factors guiding the mitigation of anthropogenic emissions to achieve the Paris climate goals.Previous studies have proposed a range of allocations of global carbon budgets,but few have quantified the equity-efficiency interaction.Based on an investigation of the existing allocation literature,this study conducts a novel analysis using a‘mixed’allocation‘big-data’framework to understand the equityeefficiency interaction in the distribution of global carbon budgets under 2℃ and 1.5℃ warming targets.At a global scale,a carbon Gini coefficient and aggregate abatement costs are used as quantitative metrics to reflect equity and efficiency,respectively.Results show an equity-efficiency frontier that reflects the opportunity for the international community to co-improve equity and efficiency on top of existing allocations.However,the frontier also features strong trade-offs to further improve equity and efficiency if national allocations are to be achieved individually.Our analysis verifies that such trade-offs are sensitively dependent on the level of global connection and integration.Linking national mitigation actions and potentials can help promote equity-efficiency synergies and contribute to the efficient achievement of the Paris Agreement's temperature and equity goals.展开更多
基金This work was fully supported by the Indonesian Endowment Fund for Education and the Indonesian Science Fund through the International Collaboration RISPRO Funding Program(No.RISPRO/KI/B1/KOM/11/4542/2/2020).
文摘Controlled C-N configurations,i.e.,pyrrolic-N,pyridinic-N,and graphitic-N,are promising strategies to tailor the carbon dots’(CDs)optical properties into the first near infrared(NIR)window(650-900 nm),a responsive range for biomedical application.However,a deep understanding of the role of the C-N configuration in the CDs’properties is still challenging and thoughtprovoking owing to their complex structure.Here,an underlying pyrrolic-N concentration and position effect on the pyrrolic-N-rich CDs’absorption was comprehensively elucidated based on the integrated experimental and computational studies.The assynthesized pyrrolic-N-rich CDs exhibit a first NIR window absorption centered at 650 nm with high photothermal conversion.Pyrrolic-N concentrations from 1.4%to 11.3%and positions(edge and mid-site)were systematically investigated.A mid-site pyrrolic-N was subsequently generated after the pyrrolic-N concentration more than 10%.Edge-site pyrrolic-N induces a frontier orbital hybridization,reducing bandgap energy,while mid-site pyrrolic-N plays a critical role in inducing a first NIR window absorption owing to their high charge transfer.Also,pyrrolic-N-rich CDs inherit a bowl-like topological feature,elevating the CDs’layer thickness as much as 0.71 nm.This study shed light on the design and optimization of pyrrolic-N on CDs for the first NIR window responsive materials in any biomedical application.
基金supported by the National Key R&D Program of China(2017YFA0605302)the National Natural Science Foundation of China(72174105).
文摘Equity and efficiency are two important factors guiding the mitigation of anthropogenic emissions to achieve the Paris climate goals.Previous studies have proposed a range of allocations of global carbon budgets,but few have quantified the equity-efficiency interaction.Based on an investigation of the existing allocation literature,this study conducts a novel analysis using a‘mixed’allocation‘big-data’framework to understand the equityeefficiency interaction in the distribution of global carbon budgets under 2℃ and 1.5℃ warming targets.At a global scale,a carbon Gini coefficient and aggregate abatement costs are used as quantitative metrics to reflect equity and efficiency,respectively.Results show an equity-efficiency frontier that reflects the opportunity for the international community to co-improve equity and efficiency on top of existing allocations.However,the frontier also features strong trade-offs to further improve equity and efficiency if national allocations are to be achieved individually.Our analysis verifies that such trade-offs are sensitively dependent on the level of global connection and integration.Linking national mitigation actions and potentials can help promote equity-efficiency synergies and contribute to the efficient achievement of the Paris Agreement's temperature and equity goals.
