Excessive consumption of energy and resources is a major challenge in wastewater treatment.Here,a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphenelike catalysts (Cu-GCD NSs) was first synthesiz...Excessive consumption of energy and resources is a major challenge in wastewater treatment.Here,a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphenelike catalysts (Cu-GCD NSs) was first synthesized by an enhanced carbothermal reduction of β-cyclodextrin (β-CD).The catalyst exhibits excellent Fenton-like catalytic activity for the degradation of various pollutants under neutral conditions,accompanied by low H_(2)O_(2)consumption.The results of structural characterization and theoretical calculations confirmed that the dual reaction centers (DRCs) were constructed on Cu-GCD NSs surface through C-O-Cu bonds supported on zero-valent copper species,which play a significant role in the high-performance Fenton-like reaction.The pollutants that served as electron donors were decomposed in the electron-poor carbon centers,whereas H_(2)O_(2)and dissolved oxygen obtained these electrons in the electron-rich Cu centers through C-O-Cu bonds,thereby producing more active species.This study demonstrates that the electrons of pollutants can be efficiently utilized in Fenton-like reactions by DRCs on the catalyst surface,which provides an effective strategy to improve Fenton-like reactivity and reduce H_(2)O_(2)consumption.展开更多
Triggered by global water quality safety issues,the research on wastewater treatment and water purification technology has been greatly developed in recent years.The Fenton technology is particularly powerful due to t...Triggered by global water quality safety issues,the research on wastewater treatment and water purification technology has been greatly developed in recent years.The Fenton technology is particularly powerful due to the rapid attack on pollutants by the generated hydroxyl radicals(·OH).However,both heterogeneous and homogeneous Fenton/Fenton-like technologies follow the classical reaction mechanism,which depends on the oxidation and reduction of the transition metal ions at single sites.So even after a century of development,this reaction still suffers from its inherent bottlenecks in practical application.In recent years,our group has been focusing on studying a novel heterogeneous Fenton catalytic process,and we developed the dual-reaction-center(DRC)system for the first time.In the DRC system,H2O2 and O2 can be efficiently reduced to reactive oxygen species(ROS)in electron-rich centers,while pollutants are captured and oxidized by the electron-deficient centers.The obtained electrons from pollutants are diverted to the electron-rich centers through bonding bridges.This process breaks through the classic Fenton mechanism,and improves the performance and efficiency of pollutant removal in a wide pH range.Here,we provide a brief overview of Fenton's story and focus on combing the discovery and development of the DRC technology and mechanism in recent years.The construction of the DRC and its performance in the pollutant degradation and interfacial reaction process are described in detail.We look forward to bringing a new perspective to continue Fenton's story through research and development of DRC technology.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.52070046,51808140,51838005 and 21906034)the Introduced Innovative R&D Team Project under the"Pearl River Talent Recruitment Program"of Guangdong Province (No.2019ZT08L387)the BL14W1 beamline of Shanghai Synchrotron Radiation Facility (SSRF,China)。
文摘Excessive consumption of energy and resources is a major challenge in wastewater treatment.Here,a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphenelike catalysts (Cu-GCD NSs) was first synthesized by an enhanced carbothermal reduction of β-cyclodextrin (β-CD).The catalyst exhibits excellent Fenton-like catalytic activity for the degradation of various pollutants under neutral conditions,accompanied by low H_(2)O_(2)consumption.The results of structural characterization and theoretical calculations confirmed that the dual reaction centers (DRCs) were constructed on Cu-GCD NSs surface through C-O-Cu bonds supported on zero-valent copper species,which play a significant role in the high-performance Fenton-like reaction.The pollutants that served as electron donors were decomposed in the electron-poor carbon centers,whereas H_(2)O_(2)and dissolved oxygen obtained these electrons in the electron-rich Cu centers through C-O-Cu bonds,thereby producing more active species.This study demonstrates that the electrons of pollutants can be efficiently utilized in Fenton-like reactions by DRCs on the catalyst surface,which provides an effective strategy to improve Fenton-like reactivity and reduce H_(2)O_(2)consumption.
基金supported by the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme(Young Scholar)the Introduced Innovative R&D Team Project under the"Pearl River Talent Recruitment Program"of Guangdong Province(No.2019ZT08L387),the Natural Science Foundation of Guangdong Province(No.2018A030313487)+1 种基金the National Natural Science Foundation of China(Grant Nos.51808140,51838005 and 51538013)the Young Innovative Talent Project in Higher Education of Guangdong Province(No.2017KQNCX150).
文摘Triggered by global water quality safety issues,the research on wastewater treatment and water purification technology has been greatly developed in recent years.The Fenton technology is particularly powerful due to the rapid attack on pollutants by the generated hydroxyl radicals(·OH).However,both heterogeneous and homogeneous Fenton/Fenton-like technologies follow the classical reaction mechanism,which depends on the oxidation and reduction of the transition metal ions at single sites.So even after a century of development,this reaction still suffers from its inherent bottlenecks in practical application.In recent years,our group has been focusing on studying a novel heterogeneous Fenton catalytic process,and we developed the dual-reaction-center(DRC)system for the first time.In the DRC system,H2O2 and O2 can be efficiently reduced to reactive oxygen species(ROS)in electron-rich centers,while pollutants are captured and oxidized by the electron-deficient centers.The obtained electrons from pollutants are diverted to the electron-rich centers through bonding bridges.This process breaks through the classic Fenton mechanism,and improves the performance and efficiency of pollutant removal in a wide pH range.Here,we provide a brief overview of Fenton's story and focus on combing the discovery and development of the DRC technology and mechanism in recent years.The construction of the DRC and its performance in the pollutant degradation and interfacial reaction process are described in detail.We look forward to bringing a new perspective to continue Fenton's story through research and development of DRC technology.
