Hydrogen evolution reaction(HER) is crucial for achieving sustainable development and carbon neutrality, and thus demands efficient catalysts, which necessitates fundamental theory to relieve trial-and-error experimen...Hydrogen evolution reaction(HER) is crucial for achieving sustainable development and carbon neutrality, and thus demands efficient catalysts, which necessitates fundamental theory to relieve trial-and-error experiment. To fast screen HER candidates, most studies focus on d-band center(ε)associated with the Gibbs energy of H* adsorption(ΔG). Unfortunately, εrule is not applicable to Pt single atoms on transition metal disulfides(Pt_(1)/TMDs) because of the additional contributions from p states of S atom. Here, we propose a new HER descriptor — d-band frontier(d) by defining the weight of d-band in the energy range of [-1.0 eV, 1.0 eV] of Pt single atoms. This dis exactly correlated with the ΔGof Pt_(1)/TMDs, and thus perfectly describes the structure–activity relationship, as validated by systematical experimental evidences. Moreover, this ddescriptor can be extended to Pt single atoms anchored on other supports(e.g., CN, C, MoO, and CoO), indicating its promising generality.展开更多
It is commonly known that the performance of electrocatalysts is largely influenced by the size,morphology,composition,and crystalline phase of noble metal nanocrystals.However,the limited reserves and high cost of no...It is commonly known that the performance of electrocatalysts is largely influenced by the size,morphology,composition,and crystalline phase of noble metal nanocrystals.However,the limited reserves and high cost of noble metals largely restrict their industrial applications.Along with the development of characterization techniques,theoretical calculations,and advanced material synthesis methods,modulating the electrocatalytic properties of noble metal nanocrystals at the atomic scale(e.g.,monolayer/sub-monolayer,single-atom alloy,ultrafine structure)has been flooding out.Engineering noble metal nanocrystals at the atomic level could not only immensely improve the noble metal atom utilization efficiency and lower the cost,but also boost the catalytic performance.In this review,we summarize the recent advanced progresses of regulating the noble metal nanocrystals at the atomic scale towards energy conversion application.Then,the challenges and perspectives of designing noble metal nanocrystals at the atomic scale in the future are discussed and considered.It is expected that this review will inspire scientists to further study precious metal-based materials for energy-oriented catalysis.展开更多
Bacterial infection arised from multipathogenic bacteria is a tricky issue that attracts worldwide attentions.In this paper,a highly accessible copper single-atom catalyst(Cu SAC)supported by biocompatible N-doped mes...Bacterial infection arised from multipathogenic bacteria is a tricky issue that attracts worldwide attentions.In this paper,a highly accessible copper single-atom catalyst(Cu SAC)supported by biocompatible N-doped mesoporous carbon nanospheres was synthesized with the emulsion-template method.The tightly anchored copper single-atom of the catalyst could effectively transform O_(2) into O_(2)−•under ambient conditions by the ultra-large pore size(~23.80 nm)and small particle size(~97.71 nm).Due to multiple synergistically oxidative damages to biomolecules,the Cu SAC could be employed to eliminate different bacteria in vitro without the generation of multidrug resistance(MDR).Moreover,the Cu SAC could also promote wound healing in vivo by eradicating the propagation of bacteria at wound.It is envisioned that the Cu SAC with superior antibacterial performance could be applied in the treatment of related bacterial infection in future.展开更多
Nitrate(NO_(3)^(-)),as a typical contaminant that can cause eutrophication,disturb the natural nitrogen cycle and pose a great risk to human health,is widely distributed in various wastewaters,such as industrial,texti...Nitrate(NO_(3)^(-)),as a typical contaminant that can cause eutrophication,disturb the natural nitrogen cycle and pose a great risk to human health,is widely distributed in various wastewaters,such as industrial,textile,and polluted ground wastewater[1].展开更多
基金supported by the National Natural Science Foundation of China(21872061,22102100)an the National Key Research and Development Program of China(2018YFC1800801)。
文摘Hydrogen evolution reaction(HER) is crucial for achieving sustainable development and carbon neutrality, and thus demands efficient catalysts, which necessitates fundamental theory to relieve trial-and-error experiment. To fast screen HER candidates, most studies focus on d-band center(ε)associated with the Gibbs energy of H* adsorption(ΔG). Unfortunately, εrule is not applicable to Pt single atoms on transition metal disulfides(Pt_(1)/TMDs) because of the additional contributions from p states of S atom. Here, we propose a new HER descriptor — d-band frontier(d) by defining the weight of d-band in the energy range of [-1.0 eV, 1.0 eV] of Pt single atoms. This dis exactly correlated with the ΔGof Pt_(1)/TMDs, and thus perfectly describes the structure–activity relationship, as validated by systematical experimental evidences. Moreover, this ddescriptor can be extended to Pt single atoms anchored on other supports(e.g., CN, C, MoO, and CoO), indicating its promising generality.
基金supported by the National Key R&D Program of China 2017YFA(0208300,0700104)the National Natural Science Foundation of China(21522107,21671180)+1 种基金the DNL Cooperation Fund,CAS(NDL201918)the China Postdoctoral Science Foundation(2019TQ0295,2019M662165)。
文摘It is commonly known that the performance of electrocatalysts is largely influenced by the size,morphology,composition,and crystalline phase of noble metal nanocrystals.However,the limited reserves and high cost of noble metals largely restrict their industrial applications.Along with the development of characterization techniques,theoretical calculations,and advanced material synthesis methods,modulating the electrocatalytic properties of noble metal nanocrystals at the atomic scale(e.g.,monolayer/sub-monolayer,single-atom alloy,ultrafine structure)has been flooding out.Engineering noble metal nanocrystals at the atomic level could not only immensely improve the noble metal atom utilization efficiency and lower the cost,but also boost the catalytic performance.In this review,we summarize the recent advanced progresses of regulating the noble metal nanocrystals at the atomic scale towards energy conversion application.Then,the challenges and perspectives of designing noble metal nanocrystals at the atomic scale in the future are discussed and considered.It is expected that this review will inspire scientists to further study precious metal-based materials for energy-oriented catalysis.
基金This work was supported by National Key R&D Program of China 2017YFA(Nos.0208300 and 0700104)the National Natural Science Foundation of China(No.21671180)We thank the funding support from CAS Fujian Institute of Innovation.This work was financially supported by the Cooperation Fund(No.DNL201918)。
文摘Bacterial infection arised from multipathogenic bacteria is a tricky issue that attracts worldwide attentions.In this paper,a highly accessible copper single-atom catalyst(Cu SAC)supported by biocompatible N-doped mesoporous carbon nanospheres was synthesized with the emulsion-template method.The tightly anchored copper single-atom of the catalyst could effectively transform O_(2) into O_(2)−•under ambient conditions by the ultra-large pore size(~23.80 nm)and small particle size(~97.71 nm).Due to multiple synergistically oxidative damages to biomolecules,the Cu SAC could be employed to eliminate different bacteria in vitro without the generation of multidrug resistance(MDR).Moreover,the Cu SAC could also promote wound healing in vivo by eradicating the propagation of bacteria at wound.It is envisioned that the Cu SAC with superior antibacterial performance could be applied in the treatment of related bacterial infection in future.
基金supported by the National Natural Science Foundation of China(21872061 and 22102100)the Natural Science Foundation of Shanghai(22ZR1431700)the National Key Research and Development Program of China(2018YFC1800801)。
文摘Nitrate(NO_(3)^(-)),as a typical contaminant that can cause eutrophication,disturb the natural nitrogen cycle and pose a great risk to human health,is widely distributed in various wastewaters,such as industrial,textile,and polluted ground wastewater[1].