Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrent...Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrently construct heterogeneous interfaces,adjust phase structure,and regulate electronic configuration,thereby enhancing OER performance.Thanks to the role of CeO_(2)coupling in reducing the activation-energy and accelerating the reaction kinetics,the heterogeneous NixSey/CeO_(2)catalyst exhibits a low overpotential of 218 mV at 10 mA/cm2and long-term stability(>400 h)in 1.0 mol/L KOH for OER.Moreover,the post-OER characterization reveals that the NixSeymatrix is reconstructed into NiOOH,while the incorporated CeO_(2)nanocrystals self-assemble into larger polycrystalline particles.Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO_(2)interfaces can modulate intermediate chemisorption toward favorable OER kinetics.This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO_(2)-coupled electrocatalysts.展开更多
Recently,metal selenides have obtained widespread attention as electrode materials for alkali(Li^(+)/Na^(+)/K^(+))batteries due to their promising theoretical capacity and mechanism.Nevertheless,metal selenides,simila...Recently,metal selenides have obtained widespread attention as electrode materials for alkali(Li^(+)/Na^(+)/K^(+))batteries due to their promising theoretical capacity and mechanism.Nevertheless,metal selenides,similar to metal oxides and sulfides,also suffer from severe volume explosion during repeated charge/discharge processes,which results in the structure collapse and the following pulverization of electrode materials.Hence,it leads to poor cycle stability and influencing their further application.In order to solve these issues,some special strategies,including elemental doping,coupling with carbon materials,synthesis of the bimetal selenides with heterostructure,etc.,have been gradually applied to design novel electrode materials with outstanding electrochemical performance.Herein,the recent research progress on metal selenides as anodes for alkali ion batteries is summarized,including the regulation of crystal structure,synthesis strategies,modification methods,and electrochemical mechanisms and kinetics.Besides,the challenges of metal selenides and the perspective for future electrode material design are proposed.It is hoped to pave a way for the development of metal selenide electrode materials for the potential applications for alkali metal ion(Li^(+)/Na^(+)/K^(+))batteries.展开更多
Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conduc...Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conductivity of active material and shuttling effect of lithium polysulfides(LiPSs)limit the commercial development of LSBs.To solve these problems,we design a core-shell composite with nitrogen-doped carbon(NC)and two types of selenides(FeSe_(2)-NC@ZnSe-NC).The FeSe_(2)-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb LiPSs.At the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction processes.The mechanism involved in FeSe_(2)-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory(DFT)calculations.The electrochemical test results indicate that LSB with S/FeSe_(2)-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g^(-1)at 0.2C.And after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe_(2)-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.展开更多
尿素氧化反应(UOR)是一种很有前途的可再生能源生产技术,为电解水制氢提供了有效的替代方案,因此开发高效稳定的UOR催化剂至关重要。本文通过NaBH4还原和硒化策略合成了富含Co、Mn和Mo的硒化镍催化剂(NiCoMnMoSe),该催化剂具有球形纳米...尿素氧化反应(UOR)是一种很有前途的可再生能源生产技术,为电解水制氢提供了有效的替代方案,因此开发高效稳定的UOR催化剂至关重要。本文通过NaBH4还原和硒化策略合成了富含Co、Mn和Mo的硒化镍催化剂(NiCoMnMoSe),该催化剂具有球形纳米颗粒与纳米片共存结构。X射线光电子能谱(XPS)、紫外-可见分光光度法(UV-vis)和原位bode相图表明,Mn和Mo的协同效应调节了Ni/Co的电子结构,提高了硒化物的电导率并加速加速电荷转移动力学,从而促进Ni^(2+)/Co^(2+)快速转变为活性Ni^(3+)/Co^(3+),并显著降低了NiCoMnMo-Se的起始电位。在UOR过程中,大部分Mo和Se被氧化成钼酸盐和硒酸盐溶解在电解质中,暴露出更多的Ni(Co)OOH活性位点,从而加快UOR反应。另外,Mn的引入稳固了活性位点,极大地增强催化剂的整体稳定性。正如预期的那样,NiCoMnMo-Se催化剂在UOR过程中表现出优异的电催化和稳定性性能,在仅1.38 V vs.RHE(相对于可逆氢电极)的电位下实现了50 mA·cm^(−2)的电流密度,并在50 mA·cm^(−2)电流密度下运行50 h后电压仅上升3.0%。当NiCoMnMo-Se和商业Pt/C组装成用于碱性尿素电解的双电极体系时,它只需要1.59 V vs.RHE便达到50 mA·cm^(−2)。展开更多
Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense...Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.展开更多
Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SI...Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SIBs).In this study,WSe_(2)/MoSe_(2)nanosheets with a better-matched and stable heterojunction interface were uniformly embedded in carbon nanofiber frameworks(WSe_(2)/MoSe_(2)/CNFs).The ion/electron transfer kinetics were facilitated by heterointerfaces with an enlarged effective utilization range.Meanwhile,the heterointerface directed electron transfer from MoSe_(2)to WSe_(2)and had significant potassium adsorption capability.The ultra-high pseudocapacitance contribution originating from the heterostructure and morphological features of the WSe_(2)/MoSe_(2)nanosheets contributed to enhancing high-rate energy storage.Moreover,in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy revealed the potassification/depotassification behavior of the WSe_(2)/MoSe_(2)/CNFs during the conversion reaction.Consequently,after 500 cycles at 5 A·g^(-1),the WSe_(2)/MoSe_(2)/CNF anode demonstrated an outstanding long-term cycling performance of 125.6 mAh·g^(-1)for PIBs.While serving as a SIB electrode,it exhibited an exceptional rate capability of 243.5 mAh·g^(-1)at 20 A·g^(-1).With the goal of developing high-performance PIB/SIB electrode materials,the proposed strategy,based on heterointerface adaptation engineering,is promising.展开更多
Flexible tandem solar cells,promising for lightweight power generation,face a hurdle:getting high-quality layers to stick well to rough surfaces like copper indium gallium selenide(CIGS).Scientists have now developed ...Flexible tandem solar cells,promising for lightweight power generation,face a hurdle:getting high-quality layers to stick well to rough surfaces like copper indium gallium selenide(CIGS).Scientists have now developed an innovative strategy to improve this,significantly boosting cell performance and durability.展开更多
Transition metal selenides(TMSs)are effective pre-electrocatalysts and are commonly used in electrochemical processes.During the electrocatalytic oxygen evolution reaction(OER),metal cations in TMSs are in-situ recons...Transition metal selenides(TMSs)are effective pre-electrocatalysts and are commonly used in electrochemical processes.During the electrocatalytic oxygen evolution reaction(OER),metal cations in TMSs are in-situ reconstructed and converted into high-valence metal oxyhydroxides.However,a limited understanding of the effects of electro-oxidation and anion leaching has resulted in insufficient theoretical guidance for the rational design of efficient catalysts.Herein,FeSe@NiSe nanorods were fabricated for the OER using a facile hydrothermal selenization method supported on FeNi foam.In-situ Raman spectroscopy and multiple characterization techniques were employed to elucidate the mechanism of FeSe@NiSe surface evolution.Metal cations on the catalyst surface were reconstructed and converted into OER-active species Fe/NiOOH at low potential.As the applied potential increased,electro-oxidation and leaching of Se occurred,resulting in SeO_(4)^(2−)adsorption on the catalyst surface,which further enhanced catalytic activity.As a result,the reconstructed FeSe@NiSe/iron-nickel foam(INF)exhibited exceptional catalytic activity for OER,achieving an ultralow overpotential of 283 mV at a current density of 100 mA·cm^(−2).Notably,the bifunctional FeSe@NiSe/INF electrode facilitated overall water splitting,affording a current density of 10 mA·cm^(−2) only at 1.53 V,even superior to the noble RuO_(2)(+)||Pt/C(−).This work offers valuable insights into the surface evolution and electrocatalytic mechanisms of TMSs.展开更多
Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary ba...Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.展开更多
With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains a...With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains an important challenge.An incipient wetness impregnation method followed by in-situ selenization was used to load copper selenide(CuSe) onto the surface of optimal magnetic biochar (OMBC).The results showed that CuSe significantly enhanced the Hg0removal performance of the OMBC,and CuSe loading ratio of 10%(10CuSe/OMBC) had the best Hg0removal performance.10CuSe/OMBC maintained its Hg0removal efficiency above 95% for 150 min at 30-150℃,and it had a good resistance to SO2.The equilibrium adsorption capacity of 10CuSe/OMBC could reach up to 8.73 mg/g,which was close to the theoretical value 12.99 mg/g,and the adsorption rate was up to 20.33μg/(g·min) Meanwhile,10CuSe/OMBC had strong magnetism that is not permanently magnetized,which could be separated from desulfurization gypsum and recycled many times.Characterization results demonstrated that Se22-,Cu2+and Oβplayed essential roles in the oxidation of Hg0,and Se22-and Se2-can immobilize Hg2+to HgSe.10CuSe/OMBC has important guiding significance for practical application because of its low cost,high performance and low mercury leaching characteristic to form HgSe.展开更多
Wearable photodetectors have come under the limelight of optoelectronic technologies on account of multiple advantages spanning light weight,easy-portability,excellent bendability,outstanding conformability,etc.Among ...Wearable photodetectors have come under the limelight of optoelectronic technologies on account of multiple advantages spanning light weight,easy-portability,excellent bendability,outstanding conformability,etc.Among diverse candidate materials,low-dimensional van der Waals materials(LDvdWMs)have emerged to be preeminent owing to the dangling-bond-free surface,exceptional carrier mobility,nanoscale dimensionality,and excellent light-harvesting capability.However,to date,the majority of flexible LDvdWM photodetectors have been fabricated through exfoliation-,transfer-,or solution-processing methods,which are plagued by limitations such as low production yield,inadequate photosensitivity,and sluggish response rate.Thus far,constructing LDvdWM photodetectors in situ on flexible substrates remains quite challenging due to the irreconcilable contradiction between the weak robustness of flexible polymer substrates against high temperature and the large thermal budget required for crystallization.This study develops scalable preparation of Sb_(2)Se_(3)nanofilm directly on flexible polyimide substrates by exploiting pulsed-laser deposition(PLD),where highly energetic species can be generated to enable overcoming the reaction barrier for crystallization at a relatively low temperature.The corresponding Sb_(2)Se_(3)photodetectors have exhibited high responsivity of 1.15 A/W,exceptional external quantum efficiency of 269%,and impressive specific detectivity reaching 2.4×10^(11)Jones,coupled with swift switching characteristics.Importantly,excellent durability to repeated bending treatments has been confirmed by the consistent photoresponse over 500 convex/concave bending cycles.Furthermore,the device has showcased strong robustness against extrinsic impinging.In the end,by using Sb_(2)Se_(3)photodetectors as sensing components,wide-band imaging beyond human vision and heart rate monitoring have been realized.This study has underscored the high efficacy of PLD for reconciling the long-standing contradiction between the weak robustness of flexible polymer substrates against high temperature and the substantial thermal energy required for crystallization,opening new opportunities towards next-generation wearable optoelectronic industry.展开更多
基金supported by the grants from the National Natural Science Foundation of China(No.22202098)the Natural Science Foundation of Henan Province(No.242300420199)。
文摘Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrently construct heterogeneous interfaces,adjust phase structure,and regulate electronic configuration,thereby enhancing OER performance.Thanks to the role of CeO_(2)coupling in reducing the activation-energy and accelerating the reaction kinetics,the heterogeneous NixSey/CeO_(2)catalyst exhibits a low overpotential of 218 mV at 10 mA/cm2and long-term stability(>400 h)in 1.0 mol/L KOH for OER.Moreover,the post-OER characterization reveals that the NixSeymatrix is reconstructed into NiOOH,while the incorporated CeO_(2)nanocrystals self-assemble into larger polycrystalline particles.Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO_(2)interfaces can modulate intermediate chemisorption toward favorable OER kinetics.This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO_(2)-coupled electrocatalysts.
基金supported by the National Natural Science Foundation of China(Nos.51563002 and 52101243)the"100-level"Innovative Talents Project of Guizhou Province,China(No.[2016]5653)+1 种基金the Natural Science Foundation of Guangdong Province(No.2020A1515010886)the Science and Technology Planning Project of Guangzhou(No.202102010373)。
文摘Recently,metal selenides have obtained widespread attention as electrode materials for alkali(Li^(+)/Na^(+)/K^(+))batteries due to their promising theoretical capacity and mechanism.Nevertheless,metal selenides,similar to metal oxides and sulfides,also suffer from severe volume explosion during repeated charge/discharge processes,which results in the structure collapse and the following pulverization of electrode materials.Hence,it leads to poor cycle stability and influencing their further application.In order to solve these issues,some special strategies,including elemental doping,coupling with carbon materials,synthesis of the bimetal selenides with heterostructure,etc.,have been gradually applied to design novel electrode materials with outstanding electrochemical performance.Herein,the recent research progress on metal selenides as anodes for alkali ion batteries is summarized,including the regulation of crystal structure,synthesis strategies,modification methods,and electrochemical mechanisms and kinetics.Besides,the challenges of metal selenides and the perspective for future electrode material design are proposed.It is hoped to pave a way for the development of metal selenide electrode materials for the potential applications for alkali metal ion(Li^(+)/Na^(+)/K^(+))batteries.
基金financially supported by the National Natural Science Foundation of China(No.52130101)the Project of Science and Technology Development Plan of Jilin Province in China(Nos.20210402058GH and 20220201114GX)。
文摘Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conductivity of active material and shuttling effect of lithium polysulfides(LiPSs)limit the commercial development of LSBs.To solve these problems,we design a core-shell composite with nitrogen-doped carbon(NC)and two types of selenides(FeSe_(2)-NC@ZnSe-NC).The FeSe_(2)-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb LiPSs.At the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction processes.The mechanism involved in FeSe_(2)-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory(DFT)calculations.The electrochemical test results indicate that LSB with S/FeSe_(2)-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g^(-1)at 0.2C.And after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe_(2)-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.
文摘尿素氧化反应(UOR)是一种很有前途的可再生能源生产技术,为电解水制氢提供了有效的替代方案,因此开发高效稳定的UOR催化剂至关重要。本文通过NaBH4还原和硒化策略合成了富含Co、Mn和Mo的硒化镍催化剂(NiCoMnMoSe),该催化剂具有球形纳米颗粒与纳米片共存结构。X射线光电子能谱(XPS)、紫外-可见分光光度法(UV-vis)和原位bode相图表明,Mn和Mo的协同效应调节了Ni/Co的电子结构,提高了硒化物的电导率并加速加速电荷转移动力学,从而促进Ni^(2+)/Co^(2+)快速转变为活性Ni^(3+)/Co^(3+),并显著降低了NiCoMnMo-Se的起始电位。在UOR过程中,大部分Mo和Se被氧化成钼酸盐和硒酸盐溶解在电解质中,暴露出更多的Ni(Co)OOH活性位点,从而加快UOR反应。另外,Mn的引入稳固了活性位点,极大地增强催化剂的整体稳定性。正如预期的那样,NiCoMnMo-Se催化剂在UOR过程中表现出优异的电催化和稳定性性能,在仅1.38 V vs.RHE(相对于可逆氢电极)的电位下实现了50 mA·cm^(−2)的电流密度,并在50 mA·cm^(−2)电流密度下运行50 h后电压仅上升3.0%。当NiCoMnMo-Se和商业Pt/C组装成用于碱性尿素电解的双电极体系时,它只需要1.59 V vs.RHE便达到50 mA·cm^(−2)。
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing (No.06500227)the Fundamental Research Funds for the Central Universities (No.FRF-TP-22-091A1).
文摘Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.
基金supported by the National Natural Science Foundation of China(No.22201098)the Natural Science Foundation of Shandong Province(Nos.ZR2021QB005 and ZR2021MB008)Jinan City“New University 20”Project(No.202228113).
文摘Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SIBs).In this study,WSe_(2)/MoSe_(2)nanosheets with a better-matched and stable heterojunction interface were uniformly embedded in carbon nanofiber frameworks(WSe_(2)/MoSe_(2)/CNFs).The ion/electron transfer kinetics were facilitated by heterointerfaces with an enlarged effective utilization range.Meanwhile,the heterointerface directed electron transfer from MoSe_(2)to WSe_(2)and had significant potassium adsorption capability.The ultra-high pseudocapacitance contribution originating from the heterostructure and morphological features of the WSe_(2)/MoSe_(2)nanosheets contributed to enhancing high-rate energy storage.Moreover,in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy revealed the potassification/depotassification behavior of the WSe_(2)/MoSe_(2)/CNFs during the conversion reaction.Consequently,after 500 cycles at 5 A·g^(-1),the WSe_(2)/MoSe_(2)/CNF anode demonstrated an outstanding long-term cycling performance of 125.6 mAh·g^(-1)for PIBs.While serving as a SIB electrode,it exhibited an exceptional rate capability of 243.5 mAh·g^(-1)at 20 A·g^(-1).With the goal of developing high-performance PIB/SIB electrode materials,the proposed strategy,based on heterointerface adaptation engineering,is promising.
文摘Flexible tandem solar cells,promising for lightweight power generation,face a hurdle:getting high-quality layers to stick well to rough surfaces like copper indium gallium selenide(CIGS).Scientists have now developed an innovative strategy to improve this,significantly boosting cell performance and durability.
基金supported by the National Natural Science Foundation of China(No.22469018)the Natural Science Basic Research Program of Department of Science and Technology of Shaanxi Province(Nos.2023-JC-ZD-22 and 2023-JC-YB-404)the Scientific Research Startup Program for Introduced Talents of Shaanxi University of Technology(Nos.SLGRCQD2303 and SLGRCQD2306).
文摘Transition metal selenides(TMSs)are effective pre-electrocatalysts and are commonly used in electrochemical processes.During the electrocatalytic oxygen evolution reaction(OER),metal cations in TMSs are in-situ reconstructed and converted into high-valence metal oxyhydroxides.However,a limited understanding of the effects of electro-oxidation and anion leaching has resulted in insufficient theoretical guidance for the rational design of efficient catalysts.Herein,FeSe@NiSe nanorods were fabricated for the OER using a facile hydrothermal selenization method supported on FeNi foam.In-situ Raman spectroscopy and multiple characterization techniques were employed to elucidate the mechanism of FeSe@NiSe surface evolution.Metal cations on the catalyst surface were reconstructed and converted into OER-active species Fe/NiOOH at low potential.As the applied potential increased,electro-oxidation and leaching of Se occurred,resulting in SeO_(4)^(2−)adsorption on the catalyst surface,which further enhanced catalytic activity.As a result,the reconstructed FeSe@NiSe/iron-nickel foam(INF)exhibited exceptional catalytic activity for OER,achieving an ultralow overpotential of 283 mV at a current density of 100 mA·cm^(−2).Notably,the bifunctional FeSe@NiSe/INF electrode facilitated overall water splitting,affording a current density of 10 mA·cm^(−2) only at 1.53 V,even superior to the noble RuO_(2)(+)||Pt/C(−).This work offers valuable insights into the surface evolution and electrocatalytic mechanisms of TMSs.
基金funding support from the National Key Research and Development Program of China(Grant No.2020YFB0408002)the Beijing Natural Science Foundation(Z240024)+2 种基金the National Natural Science Foundation of China(Grant Nos.22279083,22461160281,W2412076)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2022B1515120006)the Central Guiding Local Science and Technology Development Special Fund Project(Grant No.ZYYD2024JD24)。
文摘Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing(No.06500227)the Fundamental Research Funds for the Central Universities(No.FRF-TP-22-091A1)+1 种基金National Natural Science Foundation of China(No.52200121),Chinese Universities Scientific Fund(No.00007713)the Guide special project(No.40103322).
文摘With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains an important challenge.An incipient wetness impregnation method followed by in-situ selenization was used to load copper selenide(CuSe) onto the surface of optimal magnetic biochar (OMBC).The results showed that CuSe significantly enhanced the Hg0removal performance of the OMBC,and CuSe loading ratio of 10%(10CuSe/OMBC) had the best Hg0removal performance.10CuSe/OMBC maintained its Hg0removal efficiency above 95% for 150 min at 30-150℃,and it had a good resistance to SO2.The equilibrium adsorption capacity of 10CuSe/OMBC could reach up to 8.73 mg/g,which was close to the theoretical value 12.99 mg/g,and the adsorption rate was up to 20.33μg/(g·min) Meanwhile,10CuSe/OMBC had strong magnetism that is not permanently magnetized,which could be separated from desulfurization gypsum and recycled many times.Characterization results demonstrated that Se22-,Cu2+and Oβplayed essential roles in the oxidation of Hg0,and Se22-and Se2-can immobilize Hg2+to HgSe.10CuSe/OMBC has important guiding significance for practical application because of its low cost,high performance and low mercury leaching characteristic to form HgSe.
基金financially supported by National Natural Science Foundation of China(Nos.U2001215,52272175,12104517)Natural Science Foundation of Guangdong Province(Nos.2022A1515011487,2021A1515110403)+1 种基金Young Top Talents Program(No.2021QN02C068)State Key Laboratory of Optoelectronic Materials and Technologies(Sun Yat-sen University).
文摘Wearable photodetectors have come under the limelight of optoelectronic technologies on account of multiple advantages spanning light weight,easy-portability,excellent bendability,outstanding conformability,etc.Among diverse candidate materials,low-dimensional van der Waals materials(LDvdWMs)have emerged to be preeminent owing to the dangling-bond-free surface,exceptional carrier mobility,nanoscale dimensionality,and excellent light-harvesting capability.However,to date,the majority of flexible LDvdWM photodetectors have been fabricated through exfoliation-,transfer-,or solution-processing methods,which are plagued by limitations such as low production yield,inadequate photosensitivity,and sluggish response rate.Thus far,constructing LDvdWM photodetectors in situ on flexible substrates remains quite challenging due to the irreconcilable contradiction between the weak robustness of flexible polymer substrates against high temperature and the large thermal budget required for crystallization.This study develops scalable preparation of Sb_(2)Se_(3)nanofilm directly on flexible polyimide substrates by exploiting pulsed-laser deposition(PLD),where highly energetic species can be generated to enable overcoming the reaction barrier for crystallization at a relatively low temperature.The corresponding Sb_(2)Se_(3)photodetectors have exhibited high responsivity of 1.15 A/W,exceptional external quantum efficiency of 269%,and impressive specific detectivity reaching 2.4×10^(11)Jones,coupled with swift switching characteristics.Importantly,excellent durability to repeated bending treatments has been confirmed by the consistent photoresponse over 500 convex/concave bending cycles.Furthermore,the device has showcased strong robustness against extrinsic impinging.In the end,by using Sb_(2)Se_(3)photodetectors as sensing components,wide-band imaging beyond human vision and heart rate monitoring have been realized.This study has underscored the high efficacy of PLD for reconciling the long-standing contradiction between the weak robustness of flexible polymer substrates against high temperature and the substantial thermal energy required for crystallization,opening new opportunities towards next-generation wearable optoelectronic industry.
