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Single‐atomic Co‐B_(2)N_(2)sites anchored on carbon nanotube arrays promote lithium polysulfide conversion in lithium-sulfur batteries 被引量:1
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作者 Zhifeng Wang Yajing Yan +8 位作者 Yongguang Zhang Yanxu Chen Xianyun Peng Xin Wang Weimin Zhao Chunling Qin Qian liu xijun liu Zhongwei Chen 《Carbon Energy》 SCIE EI CAS CSCD 2023年第11期31-43,共13页
Due to low cost,high capacity,and high energy density,lithium–sulfur(Li–S)batteries have attracted much attention;however,their cycling performance was largely limited by the poor redox kinetics and low sulfur utili... Due to low cost,high capacity,and high energy density,lithium–sulfur(Li–S)batteries have attracted much attention;however,their cycling performance was largely limited by the poor redox kinetics and low sulfur utilization.Herein,predicted by density functional theory calculations,single‐atomic Co‐B2N2 site‐imbedded boron and nitrogen co‐doped carbon nanotubes(SA‐Co/BNC)were designed to accomplish high sulfur loading,fast kinetic,and long service period Li–S batteries.Experiments proved that Co‐B2N2 atomic sites can effectively catalyze lithium polysulfide conversion.Therefore,the electrodes delivered a specific capacity of 1106 mAh g−1 at 0.2 C after 100 cycles and exhibited an outstanding cycle performance over 1000 cycles at 1 C with a decay rate of 0.032%per cycle.Our study offers a new strategy to couple the combined effect of nanocarriers and single‐atomic catalysts in novel coordination environments for high‐performance Li–S batteries. 展开更多
关键词 carbon nanotubes coordination environment engineering density functional theory calculation lithium-sulfur batteries single‐atom catalys
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Heterostructured bimetallic phosphide nanowire arrays with latticetorsion interfaces for efficient overall water splitting
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作者 Hua Zhang Hongyi Li +7 位作者 Yintang Zhou Fang Tan Ruijie Dai xijun liu Guangzhi Hu Laiming Jiang Anran Chen Renbing Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第2期420-427,I0011,共9页
Designing cost-effective and high-efficiency electrocatalysts is critical to the water splitting performance during hydrogen generation.Herein,we have developed Fe_(2)P-Co_(2)P heterostructure nanowire arrays with exc... Designing cost-effective and high-efficiency electrocatalysts is critical to the water splitting performance during hydrogen generation.Herein,we have developed Fe_(2)P-Co_(2)P heterostructure nanowire arrays with excellent lattice torsions and grain boundaries for highly efficient water splitting.According to the microstructural investigations and theoretical calculations,the lattice torsion interface not only contributes to the exposure of more active sites but also effectively tunes the adsorption energy of hydrogen/oxygen intermediates via the accumulation of charge redistribution.As a result,the Fe_(2)P-Co_(2)P heterostructure nanowire array exhibits exceptional bifunctional catalytic activity with overpotentials of 65 and 198 mV at 10 mA cm^(-2) for hydrogen and oxygen evolution reactions,respectively.Moreover,the Fe_(2)P-Co_(2)P/NF-assembled electrolyzer can deliver 10 mA cm^(-2) at an ultralow voltage of1.51 V while resulting in a high solar-to-hydrogen conversion efficiency of 19.8%in the solar-driven water electrolysis cell. 展开更多
关键词 Transition metal phosphide Lattice torsion Heterogeneous interfaces Water splitting Theoretical calculation
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Au nanoclusters anchored on TiO_(2) nanosheets for high-efficiency electroreduction of nitrate to ammonia
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作者 Miaosen Yang Tianran Wei +5 位作者 Jia He Qian liu Ligang Feng Hongyi Li Jun Luo xijun liu 《Nano Research》 SCIE EI CSCD 2024年第3期1209-1216,共8页
Electrocatalytic nitrate reduction reaction(NO_(3)RR)offers a unique rationale for green NH_(3) synthesis,yet the lack of high-efficiency NO_(3)RR catalysts remains a great challenge.In this work,we show that Au nanoc... Electrocatalytic nitrate reduction reaction(NO_(3)RR)offers a unique rationale for green NH_(3) synthesis,yet the lack of high-efficiency NO_(3)RR catalysts remains a great challenge.In this work,we show that Au nanoclusters anchored on TiO_(2) nanosheets can efficiently catalyze the conversion of NO_(3)RR-to-NH_(3) under ambient conditions,achieving a maximal Faradic efficiency of 91%,a peak yield rate of 1923μg·h^(-1)·mgcat.-1,and high durability over 10 consecutive cycles,all of which are comparable to the recently reported metrics(including transition metal and noble metal-based catalysts)and exceed those of pristine TiO_(2).Moreover,a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed,which shows a power density of 3.62 mW·cm^(-2) and a yield rate of 452μg·h^(-1)·mgcat.-1.Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO_(3)-species,and reduce the NO_(3)RR-to-NH_(3) barrier,thus leading to an accelerated cathodic reaction.This work highlights the importance of metal clusters for the NH_(3) electrosynthesis and nitrate removal. 展开更多
关键词 NH3 electrosynthesis Zn-nitrate battery Au nanoclusters nitrate reduction reaction(NRR) TiO_(2)nanosheets
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Hot subduction in the southern Paleo-Asian Ocean:Insights from clinopyroxene chemistry and Sr-Nd-Hf-Pb isotopes of Carboniferous volcanics in West Junggar
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作者 Yao Xiao xijun liu +5 位作者 Wenjiao Xiao Xiao-Han Gong Hao Wu Yujia Song Zhiguo Zhang Pengde liu 《Geoscience Frontiers》 SCIE CAS CSCD 2024年第1期155-174,共20页
The chemical evolution and pressure-temperature conditions of subduction zone magmatism along ancient suture zones in orogenic belts can provide important information regarding plate convergence processes in paleo-oce... The chemical evolution and pressure-temperature conditions of subduction zone magmatism along ancient suture zones in orogenic belts can provide important information regarding plate convergence processes in paleo-oceans.Carboniferous magmatism in West Junggar is key to understanding the tectonothermal and subduction history of the Junggar Ocean,which was a branch of the Paleo-Asian Ocean,as well as the accretionary processes in the southwestern Central Asian Orogenic Belt(CAOB).We undertook a geochronological,mineralogical,geochemical,and Sr-Nd-Hf-Pb isotopic study of volcanic rocks from the Baikouquan area of West Junggar.We used these data to determine the petrogenesis,mantle source,and pressure-temperature conditions of these magmas,and further constrain the subduction and tectonic history of the Junggar Ocean.The studied volcanic rocks yielded zircon U-Pb ages of 342-337 Ma and are characterized by enrichments of large-ion lithophile elements(LILEs),and depletions in high-field-strength elements(HFSEs),indicative of an island arc affinity.The volcanic rocks have positiveƐNd(t)(5.83-7.04)andƐHf(t)(13.47-15.74)values,87Sr/86Sr(t)ratios of 0.704023-0.705658,and radiogenic 207Pb/204Pb(t)and 208Pb/204Pb(t)ratios at a given 206Pb/204Pb(t)ratio,indicative of a depleted mantle source contaminated by subduction-related materials.Geochemical modeling calculations indicate that≤1%of a subduction component comprising fluid and sediment melt could have generated the source of the parental melts of the Baikouquan volcanic rocks.Clinopyroxene phenocrysts in the volcanic rocks are classified as high-and low-Ti clinopyroxene,and pressure-temperature calculations suggest the host rocks formed at high temperatures(~1300℃)and shallow to moderate depths(<2 GPa).The magma was probably generated by hot and hydrous melting in a mantle wedge in response to subduction of young,hot oceanic lithosphere.The present results,combined with published data,suggest that the Baikouquan volcanic rocks record a transition in tectonic setting from normal cold to anomalous hot subduction of young oceanic lithosphere close to a mid-ocean ridge.This indicates ridge subduction began shortly after 337 Ma.Our results provide new insights into the tectonomagmatic evolution during intra-oceanic subduction prior to ridge subduction. 展开更多
关键词 Hot subduction Sr-Nd-Hf-Pb isotopes Clinopyroxene chemistry West Junggar Central Asian Orogenic Belt
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Coupling Co-Ni phosphides for energy-saving alkaline seawater splitting
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作者 Weijia liu Wenxian liu +7 位作者 Tong Hou Junyang Ding Zhigui Wang Ruilian Yin Xingyuan San Ligang Feng Jun Luo xijun liu 《Nano Research》 SCIE EI CSCD 2024年第6期4797-4806,共10页
The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction(HER)in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion... The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction(HER)in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion issues.However,the fabrication of efficient multifunctional catalysts for this promising technology is of great challenge.Herein,a heterostructured catalyst comprising CoP and Ni_(2)P on nickel foam(CoP/Ni_(2)P@NF)is reported for hydrazine oxidation(HzOR)-assisted alkaline seawater splitting.The coupling of CoP and Ni_(2)P optimizes the electronic structure of the active sites and endows excellent electrocatalytic performance for HzOR and HER.Impressively,the two-electrode HzOR-assisted alkaline seawater splitting(OHzS)cell based on the CoP/Ni_(2)P@NF required only 0.108 V to deliver 100 mA·cm^(−2),much lower than 1.695 V for alkaline seawater electrolysis cells.Moreover,the OHzS cell exhibits satisfactory stability over 48 h at a high current density of 500 mA·cm^(−2).Furthermore,the CoP/Ni_(2)P@NF heterostructured catalyst also efficiently catalyzed glucose oxidation,methanol oxidation,and urea oxidation in alkaline seawater electrolytes.This work paves a path for high-performance heterostructured catalyst preparation for energy-saving seawater electrolysis for H_(2) production. 展开更多
关键词 seawater splitting HETEROSTRUCTURE ELECTROCATALYSIS hydrazine oxidation reaction hydrogen evolution reaction
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Multi-functional layered double hydroxides supported by nanoporous gold toward overall hydrazine splitting
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作者 Yongji Qin Huijie Cao +8 位作者 Qian liu Shaoqing Yang Xincai Feng Hao Wang Meiling Lian Dongxing Zhang Hua Wang Jun Luo xijun liu 《Frontiers of Chemical Science and Engineering》 SCIE EI CSCD 2024年第1期61-69,共9页
Layered double hydroxides have demonstrated great potential for the oxygen evolution reaction,which is a crucial half-reaction of overall water splitting.However,it remains challenging to apply layered double hydroxid... Layered double hydroxides have demonstrated great potential for the oxygen evolution reaction,which is a crucial half-reaction of overall water splitting.However,it remains challenging to apply layered double hydroxides in other electrochemical reactions with high efficiency and stability.Herein,we report two-dimensional multifunctional layered double hydroxides derived from metalorganic framework sheet precursors supported by nanoporous gold with high porosity,which exhibit appealing performances toward oxygen/hydrogen evolution reactions,hydrazine oxidation reaction,and overall hydrazine splitting.The as-prepared catalyst only requires an overpotential of 233 mV to reach 10 mA·cm^(-2) toward oxygen evolution reaction.The overall hydrazine splitting cell only needs a cell voltage of 0.984 V to deliver 10 mA·cm^(-2),which is far more superior than that of the overall water splitting system(1.849 V).The appealing performances of the catalyst can be contributed to the synergistic effect between the metal components of the layered double hydroxides and the supporting effect of the nanoporous gold substrate,which could endow the sample with high surface area and excellent conductivity,resulting in superior activity and stability. 展开更多
关键词 layered double hydroxide oxygen evolution reaction hydrazine oxidation reaction overall hydrazine splitting hydrogen production
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Active-site and interface engineering of cathode materials for aqueous Zn–gas batteries 被引量:1
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作者 Wenxian liu Jinxiu Feng +5 位作者 Tianran Wei Qian liu Shusheng Zhang Yang Luo Jun Luo xijun liu 《Nano Research》 SCIE EI CSCD 2023年第2期2325-2346,共22页
Aqueous rechargeable Zn–gas batteries are regarded as promising energy storage and conversion devices due to their high safety and inherent environmental friendliness.However,the energy efficiency and power density o... Aqueous rechargeable Zn–gas batteries are regarded as promising energy storage and conversion devices due to their high safety and inherent environmental friendliness.However,the energy efficiency and power density of Zn–gas batteries are restricted by the kinetically sluggish cathode reactions,such as oxygen evolution reaction(OER)during charging and oxygen reduction reaction(ORR)/carbon dioxide reduction reaction(CO_(2)RR)/nitrogen reduction reaction(NRR)/nitric oxide reduction reaction(NORR)during discharge.In this review,battery configurations and fundamental reactions in Zn–gas batteries are first introduced,including Zn–air,Zn-CO_(2),Zn-N_(2),and Zn-NO batteries.Afterward,recent advances in active site engineering for enhancing the intrinsic catalytic activities of cathode catalysts are summarized.Subsequently,the structure and surface regulation strategies of cathode materials for optimizing the three-phase interface and improving the performance of Zn–gas batteries are discussed.Finally,some personal perspectives for the future development of Zn–gas batteries are presented. 展开更多
关键词 Zn–gas batteries electrocatalysis single-atom catalysts chemical doping heterostructure INTERFACE
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Origin of the DUPAL anomaly in the Tethyan mantle domain and its geodynamic significance 被引量:1
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作者 xijun liu Jifeng XU +1 位作者 Wenjiao XIAO Pengde liu 《Science China Earth Sciences》 SCIE EI CAS CSCD 2023年第12期2712-2727,共16页
Mantle heterogeneity has revealed systematic differences in Pb isotopic compositions between the Indian OceanSouth Atlantic mantle in the Southern Hemisphere and the Pacific Ocean-North Atlantic mantle in the Northern... Mantle heterogeneity has revealed systematic differences in Pb isotopic compositions between the Indian OceanSouth Atlantic mantle in the Southern Hemisphere and the Pacific Ocean-North Atlantic mantle in the Northern Hemisphere.This large-scale difference in mantle isotopes in the Southern Hemisphere is known as the DUPAL anomaly,but its origin remains controversial.Based on a systematic review of the Nd-Pb isotopic evolution of the Tethyan mantle domain,this study identified the long-term presence of the DUPAL anomaly in this domain since the early Paleozoic,characterized by long-term and high mantle thorium/uranium(Th/U)ratios.By comparing the Nd-Pb isotopic compositions of the Tethyan mantle domain with the Panthalassic-Pacific mantle domain(the Paleo-Asian,Paleo-Pacific,and modern Pacific oceans),it is shown that the mantle initially had low Th/U features due to early Earth crust-mantle differentiation,with the crust having high Th/U ratios.As such,the mantle initially had uniformly low Th/U ratios that were inherited throughout the Panthalassic-Pacific mantle domain.However,the plate tectonics and continental collisions in the Tethyan domain affected its characteristics,leading to the long-term and large-scale DUPAL anomaly.During the opening of and subduction in the Tethys Ocean,Gondwanaland fragmentation and frequent continent-continent collisions led to long-term and extensive crust-mantle interactions and the continuous input of highTh/U mantle sources,which thus modified the mantle.This process formed not only the unique DUPAL anomaly in the Tethyan mantle domain,but also the Tethyan tectonic domain dominated by continental collisions.Moreover,the high DUPAL anomaly in the Proto-and Paleo-Tethyan mantle domains records the effects of mantle plumes,which might have occurred primarily during the formation of the Proto-and Paleo-Tethys oceans during the early evolution of the Tethyan domain.Therefore,the inherent coupling of mantle domain properties and plate tectonic mechanisms provides important insights for understanding plate tectonics and geodynamic processes in the Tethyan domain. 展开更多
关键词 Tethyan domain DUPAL anomaly Large low-shear-velocity provinces(LLSVPs) OPHIOLITE GEODYNAMICS
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Engineering active sites of cathodic materials for high-performance Zn-nitrogen batteries 被引量:1
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作者 Shanshan Chen Kang Lian +4 位作者 Wenxian liu Qian liu Gaocan Qi Jun Luo xijun liu 《Nano Research》 SCIE EI CSCD 2023年第7期9214-9230,共17页
As an ideal carbon-free energy carrier,ammonia plays an indispensable role in modern society.The conventional industrial synthesis of NH3 by the Haber-Bosch technique under harsh reaction conditions results in serious... As an ideal carbon-free energy carrier,ammonia plays an indispensable role in modern society.The conventional industrial synthesis of NH3 by the Haber-Bosch technique under harsh reaction conditions results in serious energy consumption and environmental pollution.Therefore,it is essential to develop NH3 synthesis tactics under benign conditions.Electrochemical synthesis of NH_(3) has the advantages of mild reaction conditions and environmental friendliness,and has become a hotspot for research in recent years.It has been reported that zinc-nitrogen batteries(ZNBs),such as Zn-N_(2),Zn-NO,Zn-NO_(3)^(-),and Zn-NO_(2)^(-)batteries,can not only reduce nitrogenous species to ammonia but also have concomitant power output.However,the common drawbacks of these battery systems are unsatisfactory power density and ammonia production.In this review,the latest progress of ZNBs including the reaction mechanism of the battery and reactor design principles is systematically summarized.Subsequently,active site engineering of cathode catalysts is discussed,including vacancy defects,chemical doping,and heterostructure engineering.Finally,some insights are provided to improve the performance of ZNBs from a practical perspective of view. 展开更多
关键词 Zn-nitrogen batteries nitrogen reduction ELECTROCATALYSIS ammonia synthesis aqueous battery
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Electrocatalytic reduction of NO to NH_(3) in ionic liquids by P-doped TiO_(2) nanotubes 被引量:1
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作者 Shangcong Zhang Qian liu +7 位作者 Xinyue Tang Zhiming Zhou Tieyan Fan Yingmin You Qingcheng Zhang Shusheng Zhang Jun Luo xijun liu 《Frontiers of Chemical Science and Engineering》 SCIE EI CSCD 2023年第6期726-734,共9页
Designing advanced and cost-effective electrocatalytic system for nitric oxide(NO)reduction reaction(NORR)is vital for sustainable NH_(3) production and NO removal,yet it is a challenging task.Herein,it is shown that ... Designing advanced and cost-effective electrocatalytic system for nitric oxide(NO)reduction reaction(NORR)is vital for sustainable NH_(3) production and NO removal,yet it is a challenging task.Herein,it is shown that phosphorus(P)-doped titania(TiO_(2))nanotubes can be adopted as highly efficient catalyst for NORR.The catalyst demonstrates impressive performance in ionic liquid(IL)-based electrolyte with a remarkable high Faradaic efficiency of 89%and NH3 yield rate of 425μg·h^(−1)·mg_(cat).^(−1),being close to the best-reported results.Noteworthy,the obtained performance metrics are significantly larger than those for N_(2) reduction reaction.It also shows good durability with negligible activity decay even after 10 cycles.Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites,thereby enhancing the NO adsorption and facilitating the desorption of ^(*)NH_(3).Moreover,the utilization of IL further suppresses the competitive hydrogen evolution reaction.This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH_(3) at a high efficiency and rate. 展开更多
关键词 nitric oxide reduction reaction electrcatalysis ammonia production phosphorus-doped titania
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Evoking robust immunogenic cell death by synergistic sonodynamic therapy and glucose depletion using Au clusters/single atoms modified TiO_(2)nanosheets
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作者 Xiuxin Lu Kun Qiao +5 位作者 Firdoz Shaik Yang Zheng Zhaoyou Chu Haisheng Qian xijun liu Weiqing Zhang 《Nano Research》 SCIE EI CSCD 2023年第7期9730-9742,共13页
Facilitated by reactive oxygen species(ROS)-involved therapies,tumor cells undergo immunogenic cell death(ICD)to stimulate long-term immunity response.However,it is hard to trigger abundant and large-scale ICD for sat... Facilitated by reactive oxygen species(ROS)-involved therapies,tumor cells undergo immunogenic cell death(ICD)to stimulate long-term immunity response.However,it is hard to trigger abundant and large-scale ICD for satisfactory cancer immunotherapy.Herein,a multifunctional sonosensitizer that consists of Au single atoms and clusters anchored on TiO_(2)nanosheets(named Au_(S/C)-TiO_(2))is reported for augmented sonodynamic therapy(SDT)and glucose depletion,which ultimately induce robust ICD due to the improved ROS generation and strong endoplasmic reticulum(ER)stress.The synergy effect between Au cluster/single atom with TiO_(2)nanosheets intensifies apoptosis and ICD pathways to inhibit 80%of tumor cells through in vivo analyses.Furthermore,immune cells in vivo analyses verify the effectiveness of Au_(S/C)-TiO_(2)sonosensitizer towards the induction of antitumor immunity.This study thus reveals that simultaneous presence of ROS generation and strong ER stress can efficiently evoke a strong ICD-mediated immune response. 展开更多
关键词 single atom cluster TITANIA sonodynamic therapy immunogenic cell death MULTIFUNCTIONAL
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Formation of active oxygen species on single-atom Pt catalyst and promoted catalytic oxidation of toluene 被引量:13
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作者 Shunzheng Zhao Yanfeng Wen +8 位作者 xijun liu Xianyun Pen Fang Lü Fengyu Gao Xizhou Xie Chengcheng Du Honghong Yi Dongjuan Kang Xiaolong Tang 《Nano Research》 SCIE EI CAS CSCD 2020年第6期1544-1551,共8页
Catalytic oxidation of toluene over noble metal catalysts is a representative reaction for elimination of volatile organic compounds(VOCs).However,to fully understand the activation of molecular oxygen and the role of... Catalytic oxidation of toluene over noble metal catalysts is a representative reaction for elimination of volatile organic compounds(VOCs).However,to fully understand the activation of molecular oxygen and the role of active oxygen species generated in this reaction is still a challenging target.Herein,MgO nanosheets and single-atom Pt loaded MgO(Pt SA/MgO)nanosheets were synthesized and used as catalysts in toluene oxidation.The activation process of molecular oxygen and oxidation performance on the two catalysts were contrastively investigated.The Pt SA/MgO exhibited significantly enhanced catalytic activity compared to MgO.The oxygen vacancies can be easily generated on the Pt SA/MgO surface,which facilitate the activation of molecular oxygen and the formation of active oxygen species.Based on the experimental data and theoretical calculations,an active oxygen species promoted oxidation mechanism for toluene was proposed.In the presence of H2O,the molecular oxygen is more favorable to be dissociated to generate•OH on the oxygen vacancies of the Pt SA/MgO surface,which is the dominant active oxygen species.We anticipate that this work may shed light on further investigation of t10.1007/s12274-020-2765-1he oxidation mechanism of toluene and other VOCs over noble metal catalysts. 展开更多
关键词 single-atom Pt activation of molecular oxygen oxygen vacancies active oxygen species oxidation of toluene
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Atomic Fe-Zn dual-metal sites for high-efficiency pH-universal oxygen reduction catalysis 被引量:6
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作者 Jie Xu Shuhua Lai +15 位作者 Defeng Qi Min Hu Xianyun Peng Yifan liu Wei liu Guangzhi Hu Heng Xu Fan Li Chao Li Jia He Longchao Zhuo Jiaqiang Sun Yuan Qiu Shusheng Zhang Jun Luo xijun liu 《Nano Research》 SCIE EI CAS CSCD 2021年第5期1374-1381,共8页
An effective electrocatalyst being highly active in all pH range for oxygen reduction reaction(ORR)is crucial for energy conversion and storage devices.However,most of the high-efficiency ORR catalysis was reported in... An effective electrocatalyst being highly active in all pH range for oxygen reduction reaction(ORR)is crucial for energy conversion and storage devices.However,most of the high-efficiency ORR catalysis was reported in alkaline conditions.Herein,we demonstrated the preparation of atomically dispersed Fe-Zn pairs anchored on porous N-doped carbon frameworks(Fe-Zn-SA/NC),which works efficiently as ORR catalyst in the whole pH range.It achieves high half-wave potentials of 0.78,0.85 and 0.72 V in 0.1 M HClO4,0.1 M KOH and 0.1 M phosphate buffer saline(PBS)solutions,respectively,as well as respectable stability.The performances are even comparable to Pt/C.Furthermore,when assembled into a Zn-air battery,the high power density of 167.2 mWcm−2 and 120 h durability reveal the feasibility of Fe-Zn-SA/NC in real energy-related devices.Theoretical calculations demonstrate that the superior catalytic activity of Fe-Zn-SA/NC can be contributed to the lower energy barriers of ORR at the Fe-Zn-N6 centers.This work demonstrates the potential of Fe-Zn pairs as alternatives to the Pt catalysts for efficient catalytic ORR and provides new insights of dual-atom catalysts for other energy conversion related catalytic reactions. 展开更多
关键词 Fe-Zn atomic pairs oxygen reduction reaction pH-universal Zn-air battery electrocatalysis
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Two-in-one solution using insect wings to produce graphene-graphite films for efficient electrocatalysis 被引量:3
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作者 Huaiyu Li Lihan Zhang +7 位作者 Long Li Chaowen Wu Yajiao Huo Ying Chen xijun liu Xiaoxing Ke Jun Luo Gustaaf Van Tendeloo 《Nano Research》 SCIE EI CAS CSCD 2019年第1期33-39,共7页
Natural organisms contain rich elements and naturally optimized smart structures,both of which have inspired various innovative concepts and desig ns in human society.In particular,several natural organisms have been ... Natural organisms contain rich elements and naturally optimized smart structures,both of which have inspired various innovative concepts and desig ns in human society.In particular,several natural organisms have been used as element sources to synthesize low-cost and environmentally friendly electrocatalysts for the oxygen reduction reaction(ORR)in fuel cells and metal-air batteries,which are clean energy devices.However,to date,no naturally optimized smart structures have been employed in the synthesis of ORR catalysts,including graphene-based materials.Here,we demonstrate a novel strategy to synthesize graphene-graphite films(GGFs)by heating butterfly wings coated with FeCI3 in N2,in which the full power of natural organisms is utilized.The wings work not only as an element source for GGF generation but also as a porous supporting structure for effective nitrogen doping,two-dimensional spreading,and double-face exposure of the GGFs.These GGFs exhibit a half-wave potential of 0.942 V and a H2O2 yield of<0.07%for ORR electrocatalysis;these values are comparable to those for the best commercial Pt/C and all previously reported ORR catalysts in alkaline media.This two-in-one strategy is also successful with cicada and dragonfly wings,indicating that it is a universal,green,and cost-effective method for developing high-performance graphene-based materials. 展开更多
关键词 INSECT WINGS GRAPHENE GRAPHITE oxygen reduction reaction ELECTROCATALYSTS
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部分磷化双金属中心集成制备高性能三功能催化剂用于制氢和柔性锌-空气电池 被引量:3
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作者 杨淼森 刘亦帆 +3 位作者 孙甲强 张书胜 刘熙俊 罗俊 《Science China Materials》 SCIE EI CAS CSCD 2022年第5期1176-1186,共11页
开发高效且性能稳定的氧析出(OER)、氧还原(ORR)和氢析出(HER)三功能催化剂是制备能源存储与转换设备的关键.本文使用一步磷化法,在氮磷共掺杂碳基上制备了Fe Co金属合金/磷化物催化剂(Fe Co-P/PNC).该催化剂显示了良好的ORR性能,展现了... 开发高效且性能稳定的氧析出(OER)、氧还原(ORR)和氢析出(HER)三功能催化剂是制备能源存储与转换设备的关键.本文使用一步磷化法,在氮磷共掺杂碳基上制备了Fe Co金属合金/磷化物催化剂(Fe Co-P/PNC).该催化剂显示了良好的ORR性能,展现了0.86 V (vs.RHE,相对于可逆氢电极)的半波电位;在OER和HER反应中,催化剂在10 m A cm^(-2)的电流密度下的过电位分别为350和158 m V.密度泛函理论计算表明,磷在Fe Co磷化物和碳基体中皆起主导作用,使得该催化剂同时具有良好的ORR、OER和HER功能.以Fe Co-P/PNC为空气阴极组装的水系电池和柔性锌-空气电池的峰值功率密度分别为195.1和90.8 m W cm^(-2),且两种电池均具有优异的充放电性能、长寿命和高柔性.此外,自供能的整体水分解系统表现出较低的(1.71 V)工作电压以驱动10 m A cm^(-2)的电流密度,进一步证实了该催化剂出色的多功能性. 展开更多
关键词 trifunctional electrocatalyst multi-active sites alloy/phosphide hydrogen production flexible Zn-air battery
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MoC nanocrystals confined in N-doped carbon nanosheets toward highly selective electrocatalytic nitric oxide reduction to ammonia 被引量:3
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作者 Ge Meng Mengmeng Jin +5 位作者 Tianran Wei Qian liu Shusheng Zhang Xianyun Peng Jun Luo xijun liu 《Nano Research》 SCIE EI CSCD 2022年第10期8890-8896,共7页
Electrochemical nitric oxide reduction reaction(NORR)to produce ammonia(NH3)under ambient conditions is a promising alternative to the energy and carbon-intensive Haber–Bosch approach,but its performance is still imp... Electrochemical nitric oxide reduction reaction(NORR)to produce ammonia(NH3)under ambient conditions is a promising alternative to the energy and carbon-intensive Haber–Bosch approach,but its performance is still improved.Herein,molybdenum carbides(MoC)nanocrystals confined by nitrogen-doped carbon nanosheets are first designed as an efficient and durable electrocatalyst for catalyzing the reduction of NO to NH3 with maximal Faradaic efficiency of 89%±2%and a yield rate of 1,350±15μg·h^(−1)·cm^(−2) at the applied potential of−0.8 V vs.reversible hydrogen electrode(RHE)as well as high stable activity with negligible current density and NH3 yield rate decays over a 30 h continue the test.Moreover,as a proof-of-concept of Zn–NO battery,it achieves a peak power density of 1.8 mW·cm^(−2) and a large NH3 yield rate of 782±10μg·h^(−1)·cm^(−2),which are comparable to the best-reported results.Theoretical calculations reveal that the MoC(111)has a strong electronic interaction with NO molecules and thus lowering the energy barrier of the potential-determining step and suppressing hydrogen evolution kinetics.This work suggests that Mo-based materials are a powerful platform providing great opportunities to explore highly selective and active catalysts for NH3 production. 展开更多
关键词 ammonia electrosynthesis green route molybdenum carbides(MoC)nanocrystals nitric oxide reduction reaction high selectivity
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Common-Ion Effect Triggered Highly Sustained Seawater Electrolysis with Additional NaCl Production 被引量:3
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作者 Pengsong Li Shiyuan Wang +12 位作者 Imran Ahmed Samo Xingheng Zhang Zhaolei Wang Cheng Wang Yang Li Yiyun Du Yang Zhong Congtian Cheng Wenwen Xu xijun liu Yun Kuang Zhiyi Lu Xiaoming Sun 《Research》 EI CAS 2020年第1期465-473,共9页
Developing efficient seawater-electrolysis system for mass production of hydrogen is highly desirable due to the abundance of seawater.However,continuous electrolysis with seawater feeding boosts the concentration of ... Developing efficient seawater-electrolysis system for mass production of hydrogen is highly desirable due to the abundance of seawater.However,continuous electrolysis with seawater feeding boosts the concentration of sodium chloride in the electrolyzer,leading to severe electrode corrosion and chlorine evolution.Herein,the common-ion effect was utilized into the electrolyzer to depress the solubility of NaCl.Specifically,utilization of 6M NaOH halved the solubility of NaCl in the electrolyte,affording efficient,durable,and sustained seawater electrolysis in NaCl-saturated electrolytes with triple production of H_(2),O_(2),and crystalline NaCl.Ternary NiCoFe phosphide was employed as a bifunctional anode and cathode in simulative and Ca/Mg-free seawater-electrolysis systems,which could stably work under 500 mA/cm^(2) for over 100 h.We attribute the high stability to the increased Na^(+)concentration,which reduces the concentration of dissolved Cl-in the electrolyte according to the common-ion effect,resulting in crystallization of NaCl,eliminated anode corrosion,and chlorine oxidation during continuous supplementation of Ca/Mg-free seawater to the electrolysis system. 展开更多
关键词 CORROSION CHLORINE ELECTROLYTE
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ASYMPTOTICS FOR RUIN PROBABILITIES OF TWO KINDS OF DEPENDENT RISK MODELS WITH NLOD INTER-ARRIVAL TIMES 被引量:1
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作者 Yang YANG Yuebao WANG xijun liu 《Journal of Systems Science & Complexity》 SCIE EI CSCD 2011年第2期328-334,共7页
这份报纸证实为二种依赖者的无限时间的毁灭可能性的一些 asymptotic 公式冒险模型。一个风险模型把主张尺寸看作一个调制过程,并且其它处理否定地上面的 orthant 依赖者主张尺寸。在二个模型,内部到达的时间两个都被假定是否定地更低... 这份报纸证实为二种依赖者的无限时间的毁灭可能性的一些 asymptotic 公式冒险模型。一个风险模型把主张尺寸看作一个调制过程,并且其它处理否定地上面的 orthant 依赖者主张尺寸。在二个模型,内部到达的时间两个都被假定是否定地更低的 orthant 依赖者。 展开更多
关键词 风险模型 到达时间 破产概率 INTER 渐近公式 调制过程 权利要求 尺寸
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钴铁层状双金属氢氧化物空心多面体用于高效电催化二氧化碳还原 被引量:1
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作者 杨淼森 孙甲强 +4 位作者 秦永吉 杨慧 张书胜 刘熙俊 罗俊 《Science China Materials》 SCIE EI CAS CSCD 2022年第2期536-542,共7页
可再生能源驱动电催化二氧化碳还原制备高附加值化学燃料,是一种实现二氧化碳资源化的有效途径.以金属有机骨架(MOF)为模板制备的层状双金属氢氧化物空心多面体已成为当前电催化领域的热门材料.然而,该类材料的高析氢活性严重阻碍了其... 可再生能源驱动电催化二氧化碳还原制备高附加值化学燃料,是一种实现二氧化碳资源化的有效途径.以金属有机骨架(MOF)为模板制备的层状双金属氢氧化物空心多面体已成为当前电催化领域的热门材料.然而,该类材料的高析氢活性严重阻碍了其在电催化二氧化碳还原中的应用.基于此,本文报道了一种在离子液体电解液中可高效稳定电催化二氧化碳还原的钴铁层状双金属氢氧化物空心多面体(CoFe LDH/HP),其最大法拉第转换效率可达86%±3%(-0.9 V相对于可逆氢电极),且可连续电解30 h.实验结果表明此CoFe LDH/HP因其独特的空心结构可暴露更多的活性位点,从而具有更快的电催化二氧化碳还原动力学;理论计算表明CoFe LDH/HP中Co-O-Fe键有利于稳定关键中间体(*COOH)并降低相应的活化势垒.本研究可为其他层状双金属氢氧化物用于二氧化碳固定的设计提供参考. 展开更多
关键词 层状双金属氢氧化物 电催化 二氧化碳还原 法拉第 二氧化碳固定 多面体 空心结构 氢电极
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Highly dispersed Ag clusters for active and stable hydrogen peroxide production 被引量:1
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作者 Mengmeng Jin Wei liu +4 位作者 Jiaqiang Sun Xinzhong Wang Shusheng Zhang Jun Luo xijun liu 《Nano Research》 SCIE EI CSCD 2022年第7期5842-5847,共6页
The electrosynthesis of hydrogen peroxide(H2O2)from oxygen reduction reaction(ORR)via a two-electron pathway provides an appealing alternative to the energy-intensive anthraquinone route;however,the development of ORR... The electrosynthesis of hydrogen peroxide(H2O2)from oxygen reduction reaction(ORR)via a two-electron pathway provides an appealing alternative to the energy-intensive anthraquinone route;however,the development of ORR with high selectivity and durability for H2O2 production is still challenging.Herein,we demonstrate an active and stable catalyst,composing of highly dispersed Ag nanoclusters on N-doped hollow carbon spheres(NC-Ag/NHCS),which can effectively reduce O2 molecules into H2O2 with a selectivity of 89%–91%in a potential range from 0.2 to 0.7 V(vs.reversible hydrogen electrode(RHE))in acidic media.Strikingly,NC-Ag/NHCS achieve a mass activity of 27.1 A·g^(−1) and a yield rate of 408 mmol·gcat.^(−1)·h^(−1) at 0.7 V,both of which are comparable with the best-reported results.Furthermore,NC-Ag/NHCS enable catalyzing H2O2 production with a stable current density over 48-h electrolysis and only about 9.8%loss in selectivity after 10,000 cycles.Theoretical analyses indicate that Ag nanoclusters can contribute more electrons to favor the protonation of adsorbed O2,thus leading to a high H2O2 selectivity.This work confirms the great potential of metal nanocluster-based materials for H2O2 electrosynthesis under ambient conditions. 展开更多
关键词 hydrogen peroxide synthesis electrochemical route Ag nanoclusters oxygen reduction reaction ENERGY-EFFICIENT
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