Green hydrogen is urgently required for sustainable development of human beings and rational construction of heterostructures holds great promising for photocatalytic hydrogen generation.Herein,2D/2D WSe_(2)/ZnIn_(2)S...Green hydrogen is urgently required for sustainable development of human beings and rational construction of heterostructures holds great promising for photocatalytic hydrogen generation.Herein,2D/2D WSe_(2)/ZnIn_(2)S_(4) heterostructures with strong hetero-interface interaction and abundant contact were constructed via an impregnation-annealing strategy.Efficient charge transfer from ZnIn_(2)S_(4) to WSe_(2)was evidenced by transient absorption spectroscopy in crafted heterostructures owing to the tight and2D face-to-face contact.As a result,the prepared WSe_(2)/ZnIn_(2)S_(4) heterostructures exhibited boosted photocatalytic performance and a highest hydrogen evolution rate of 3.377 mmol/(g h)was achieved with an apparent quantum yield of 45.7%at 420 nm.The work not only provides new strategies to achieve efficient 2D/2D heterostructures but also paves the way for the development of green hydrogen in the future.展开更多
Numerous decision-makers in politics,science,and business worldwide have acknowledged that hydrogen H_(2) will become one of the most important energy sources of the 21st century if the desired energy transition to ca...Numerous decision-makers in politics,science,and business worldwide have acknowledged that hydrogen H_(2) will become one of the most important energy sources of the 21st century if the desired energy transition to carbon-free energy sources is to be taken seriously.Nevertheless,this transition in general and the introduction of H_(2) in particular is still progressing far too slowly.There are now countless projects worldwide,including several worth billions of US dollars,but we are still waiting for the breakthrough.There seem to be various reasons for this,not just one single or most important one.Purpose:In the overall context of global earth overheating(often downplayed as“climate change”),hydrogen H_(2) will undoubtedly play a decisive role as of now.The paper aims to identify the key challenges and propose solutions for establishing a sustainable value chain for market penetration of H_(2).Design/methodology/approach:This paper aims to shed light on the current situation using freely accessible publications from global management consultancies and the German government,as well as critical reporting.The problem of human behavior is also explained by the Novak Triangle.Findings:Most people have come to understand that anthropogenic global overheating can only be solved by new technologies(which cost money,time,and behavioral change)in production and application.Hydrogen H_(2) appears to be an essential part of the desired solution.Nevertheless,there are currently still numerous challenges and also concrete concerns worldwide,which partially cast the implementation in a questionable light.The findings suggest that establishing a demand and supply of H_(2) needs a comprehensive infrastructure,circular economy principles,and changes in consumer behavior and policy frameworks.The paper proposes solutions for addressing these challenges.Affected countries:The situation described here relates to Germany and the EU countries,but it is likely to be comparable,or at least similar,for many industrialized countries.The challenges and solutions proposed in this paper are relevant to countries worldwide that are transitioning to sustainable energy and transportation systems.Research/future/practical implications:As of 2024,it must be stated that the implementation of H_(2) is still progressing far too slowly,even in the“model country”Germany.There are still problems and stalling in many places.The biggest challenge seems to be the problem:without demand,there is no supply;without supply,there is no demand.This can then best be achieved with simple“out-of-the-box”solutions in mindset(see Novak triangle).The research implications of this paper include the need for further research on the challenges of establishing a sustainable value chain and the effectiveness of the proposed solutions.The future implications of this paper include the importance of establishing a sustainable value chain to mitigate climate change and reduce dependence on fossil fuels.The core point will become the collaboration across the entire value chain to establish a sustainable infrastructure for sustainable energy and transportation systems.Originality/value:Currently,there are virtually no scientific books that would present the overall context of the challenges.Therefore,only current surveys,market volumes,and challenges in environmental and working conditions can be described here.This paper contributes to the literature by analyzing the challenges of establishing a market model for hydrogen H_(2).The paper proposes solutions for addressing these challenges and shows difficulties.It provides valuable insights for policymakers,industry stakeholders,and researchers working towards a sustainable energy future.展开更多
The hydrolysis of MgH_(2) delivers high hydrogen capacity(15.2 wt%),which is very attractive for real-time hydrogen supply.However,the formation of a surface passivation Mg(OH)_(2) layer and the large excess of H_(2)O...The hydrolysis of MgH_(2) delivers high hydrogen capacity(15.2 wt%),which is very attractive for real-time hydrogen supply.However,the formation of a surface passivation Mg(OH)_(2) layer and the large excess of H_(2)O required to ensure complete hydrolysis are two key challenges for the MgH_(2) hydrolysis systems.Now,a low-cost method is reported to synthesize MgH_(2)@Mg(BH_(4))_(2) composite via ball-milling MgH_(2) with cheap and widely available B_(2)O_(3)(or B(OH)_(3)).By adding small amounts of B_(2)O_(3),the in-situ formed Mg(BH_(4))_(2) could significantly promote the hydrolysis of MgH_(2).In particular,the MgH_(2)–10 wt%B_(2)O_(3) composite releases 1330.7 mL·g^(−1) H_(2)(close to 80%theoretical hydrogen generation H_(2))in H_(2)O and 1520.4 mL·g^(−1) H_(2)(about 95%)in 0.5 M MgCl_(2) in 60 min at 26℃ with hydrolysis rate of 736.9 mL·g^(−1)·min^(−1) and 960.9 mL·g^(−1)·min^(−1) H_(2) during the first minute of the hydrolysis,respectively.In addition,the MgCl_(2) solution allows repeated use by filtering and exhibits high cycle stability(20 cycles),therefore leading to much reduced capacity loss caused by the excess H_(2)O.We show that by introducing B_(2)O_(3) and recycling the 0.5 M MgCl_(2) solution,the system hydrogen capacity can approach 5.9 wt%,providing a promising hydrogen generation scheme to supply hydrogen to the fuel cells.展开更多
In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts Pd...In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts Pd/carbon nanosphere(CNS),obtained via immobilization of ultrafine Pd nanoparticles onto CNS,are developed and employed for both selective H_(2)generation from HCOOH dehydrogenation and O_(2)evolution from H_(2)O_(2)decomposition.In these reactions,the highest activities for Pd/CNS-800(i.e.,calcinated at 800℃)are 2478 h−1 and 993 min^(−1)for H_(2)and O_(2)evolution,respectively.The highly efficient and selective“on-off”switch for selective H_(2)generation from HCOOH is successfully realized by pH adjustment.This novel and highly efficient nanocatalyst Pd/CNS-800 not only provides new approaches for the promising application of HCOOH and H_(2)O_(2)as economic and safe H_(2)and O_(2)carriers,respectively,for fuel cells,but also promotes the development of“on-off”switch for on-demand H_(2)evolution.展开更多
The effects of chloride salts(NaCl,MgCl2and NH4Cl)on the hydrolysis kinetics of MgH2prepared by hydridingcombustion synthesis and mechanical milling(HCS+MM)were discussed.X-ray diffraction(XRD)analyses show that high-...The effects of chloride salts(NaCl,MgCl2and NH4Cl)on the hydrolysis kinetics of MgH2prepared by hydridingcombustion synthesis and mechanical milling(HCS+MM)were discussed.X-ray diffraction(XRD)analyses show that high-purityMgH2was successfully prepared by HCS.Hydrolysis performance test results indicate that the chloride salt added during the millingprocess is favorable to the initial reaction rate and hydrogen generation yield within60min.A MgH2?10%NH4Cl composite exhibitsthe best performance with the hydrogen generation yield of1311mL/g and a conversion rate of85.69%in60min at roomtemperature.It is suggested that the chloride salts not only play as grinding aids in the milling process,but also create fresh surface ofreactive materials,favoring the hydrolysis reaction.展开更多
In this work,La-doped Mg-Ni multiphase alloys were prepared by resistance melting furnace(RMF)and then modified by high-energy ball milling(HEBM).The hydrolysis H_(2) generation kinetics/thermodynamics of prepared all...In this work,La-doped Mg-Ni multiphase alloys were prepared by resistance melting furnace(RMF)and then modified by high-energy ball milling(HEBM).The hydrolysis H_(2) generation kinetics/thermodynamics of prepared alloys in Na Cl solutions have been investigated with the help of nonlinear and linear fitting by Avrami-Erofeev and Arrhenius equations.Combining the microstructure information before and after hydrolysis and thermodynamics fitting results,the hydrolysis H_(2) generation mechanism based on nucleation&growth has been elaborated.The final H_(2) generation capacities of 0La,5La,10La and 15 La alloys are 677,653,641 and 770 m L·g^(-1)H_(2) in 240 min at291 K,respectively.While,the final H_(2) generation capacities of HEBM 0La,5La,10La and 15 La alloys are 632,824,611 and 653 m L·g^(-1)H_(2) in 20 min at 291 K,respectively.The as-cast 15La alloy and HEMB 5La alloy present the best H_(2) production rates and final H_(2) production capacities,especially the HEBM 5La can rapidly achieve high H_(2) generation capacity(670 and 824 m L·g^(-1)H_(2) )at low temperature(291 K)within short time(5 and 20 min).The difference between the H_(2) generation capacities is mainly originated from the initial nucleation rate of Mg(OH)_(2) and the subsequent processes affected by the microstructures and phase compositions of the hydrolysis alloys.Relative low initial nucleation rate and fully growth of Mg(OH)_(2) nucleus are the premise of high H_(2) generation capacity due to the hydrolysis H_(2) generation process consisted by the nucleation,growth and contacting of Mg(OH)_(2) nucleus.To utilization H_(2) by designing solid state H_(2) generators using optimized Mg-based alloys is expected to be a feasible H_(2) generation strategy at the moment.展开更多
Hydrogen peroxide(H_(2)O_(2)) is a high-demand organic chemical reagent and has been widely used in various modern industrial applications. Currently,the prominent method for the preparation of H_(2)O_(2) is the anthr...Hydrogen peroxide(H_(2)O_(2)) is a high-demand organic chemical reagent and has been widely used in various modern industrial applications. Currently,the prominent method for the preparation of H_(2)O_(2) is the anthraquinone oxidation.Unfortunately, it is not conducive to economic and sustainable development since it is a complex process and involves unfriendly environment and potential hazards. In this context, numerous approaches have been developed to synthesize H_(2)O_(2). Among them, photo/electro-catalytic ones are considered as two of the most promising manners for on-site synthesis of H_(2)O_(2). These alternatives are sustainable in that only water or O_(2) is required. Namely, water oxidation(WOR) or oxygen reduction(ORR)reactions can be further coupled with clean and sustainable energy. For photo/electro-catalytic reactions for H_(2)O_(2) generation, the design of the catalysts is extremely important and has been extensively conducted with an aim to obtain ultimate catalytic performance. This article overviews the basic principles of WOR and ORR,followed by the summary of recent progresses and achievements on the design and performance of various photo/electro-catalysts for H_(2)O_(2) generation. The related mechanisms for these approaches are highlighted from theoretical and experimental aspects. Scientific challenges and opportunities of engineering photo/electro-catalysts for H_(2)O_(2) generation are also outlined and discussed.展开更多
Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous car...Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous carbon materials composed of abundant graphene/hexagonal boron nitride(G/h-BN)heterostructures.Metal Ni powder and nanoscale h-BN sheets are used as a catalytic substrate/hard template and“nucleation seed”for the formation of the heterostructure,respectively.As-prepared G/h-BN heterostructures exhibit enhanced electrocatalytic activity toward H_(2)O_(2) generation with 86%-95%selectivity at the range of 0.45-0.75 V versus reversible hydrogen electrode(RHE)and a positive onset potential of 0.79 versus RHE(defined at a ring current density of 0.3 mA cm^(-2))in the alkaline solution.In a flow cell,G/h-BN heterostructured electrocatalyst has a H_(2)O_(2) production rate of up to 762 mmol g_(catalyst)^(-1) h^(-1) and Faradaic efficiency of over 75%during 12 h testing,superior to the reported carbon-based electrocatalysts.The density functional theory simulation suggests that the B atoms at the interface of the G/h-BN heterostructure are the key active sites.This research provides a new route to activate carbon catalysts toward highly active and selective O_(2)-to-H_(2)O_(2) conversion.展开更多
基金financially supported by the National Natural Science Foundation of China (No.52106259)the Fundamental Research Funds for the Central Universities (2024MS013)Key Research and Development Program of Shaanxi (Program No.2022LL-JB-08)。
文摘Green hydrogen is urgently required for sustainable development of human beings and rational construction of heterostructures holds great promising for photocatalytic hydrogen generation.Herein,2D/2D WSe_(2)/ZnIn_(2)S_(4) heterostructures with strong hetero-interface interaction and abundant contact were constructed via an impregnation-annealing strategy.Efficient charge transfer from ZnIn_(2)S_(4) to WSe_(2)was evidenced by transient absorption spectroscopy in crafted heterostructures owing to the tight and2D face-to-face contact.As a result,the prepared WSe_(2)/ZnIn_(2)S_(4) heterostructures exhibited boosted photocatalytic performance and a highest hydrogen evolution rate of 3.377 mmol/(g h)was achieved with an apparent quantum yield of 45.7%at 420 nm.The work not only provides new strategies to achieve efficient 2D/2D heterostructures but also paves the way for the development of green hydrogen in the future.
文摘Numerous decision-makers in politics,science,and business worldwide have acknowledged that hydrogen H_(2) will become one of the most important energy sources of the 21st century if the desired energy transition to carbon-free energy sources is to be taken seriously.Nevertheless,this transition in general and the introduction of H_(2) in particular is still progressing far too slowly.There are now countless projects worldwide,including several worth billions of US dollars,but we are still waiting for the breakthrough.There seem to be various reasons for this,not just one single or most important one.Purpose:In the overall context of global earth overheating(often downplayed as“climate change”),hydrogen H_(2) will undoubtedly play a decisive role as of now.The paper aims to identify the key challenges and propose solutions for establishing a sustainable value chain for market penetration of H_(2).Design/methodology/approach:This paper aims to shed light on the current situation using freely accessible publications from global management consultancies and the German government,as well as critical reporting.The problem of human behavior is also explained by the Novak Triangle.Findings:Most people have come to understand that anthropogenic global overheating can only be solved by new technologies(which cost money,time,and behavioral change)in production and application.Hydrogen H_(2) appears to be an essential part of the desired solution.Nevertheless,there are currently still numerous challenges and also concrete concerns worldwide,which partially cast the implementation in a questionable light.The findings suggest that establishing a demand and supply of H_(2) needs a comprehensive infrastructure,circular economy principles,and changes in consumer behavior and policy frameworks.The paper proposes solutions for addressing these challenges.Affected countries:The situation described here relates to Germany and the EU countries,but it is likely to be comparable,or at least similar,for many industrialized countries.The challenges and solutions proposed in this paper are relevant to countries worldwide that are transitioning to sustainable energy and transportation systems.Research/future/practical implications:As of 2024,it must be stated that the implementation of H_(2) is still progressing far too slowly,even in the“model country”Germany.There are still problems and stalling in many places.The biggest challenge seems to be the problem:without demand,there is no supply;without supply,there is no demand.This can then best be achieved with simple“out-of-the-box”solutions in mindset(see Novak triangle).The research implications of this paper include the need for further research on the challenges of establishing a sustainable value chain and the effectiveness of the proposed solutions.The future implications of this paper include the importance of establishing a sustainable value chain to mitigate climate change and reduce dependence on fossil fuels.The core point will become the collaboration across the entire value chain to establish a sustainable infrastructure for sustainable energy and transportation systems.Originality/value:Currently,there are virtually no scientific books that would present the overall context of the challenges.Therefore,only current surveys,market volumes,and challenges in environmental and working conditions can be described here.This paper contributes to the literature by analyzing the challenges of establishing a market model for hydrogen H_(2).The paper proposes solutions for addressing these challenges and shows difficulties.It provides valuable insights for policymakers,industry stakeholders,and researchers working towards a sustainable energy future.
基金supported by the Basic and Applied Basic Research Foundation of Guangdong Province(No.2022A1515011832 and 2021A1515110676)supported by GDAS’Project of Science and Technology Development(2022GDASZH-2022010104,2022GDASZH-2022030604-04).
文摘The hydrolysis of MgH_(2) delivers high hydrogen capacity(15.2 wt%),which is very attractive for real-time hydrogen supply.However,the formation of a surface passivation Mg(OH)_(2) layer and the large excess of H_(2)O required to ensure complete hydrolysis are two key challenges for the MgH_(2) hydrolysis systems.Now,a low-cost method is reported to synthesize MgH_(2)@Mg(BH_(4))_(2) composite via ball-milling MgH_(2) with cheap and widely available B_(2)O_(3)(or B(OH)_(3)).By adding small amounts of B_(2)O_(3),the in-situ formed Mg(BH_(4))_(2) could significantly promote the hydrolysis of MgH_(2).In particular,the MgH_(2)–10 wt%B_(2)O_(3) composite releases 1330.7 mL·g^(−1) H_(2)(close to 80%theoretical hydrogen generation H_(2))in H_(2)O and 1520.4 mL·g^(−1) H_(2)(about 95%)in 0.5 M MgCl_(2) in 60 min at 26℃ with hydrolysis rate of 736.9 mL·g^(−1)·min^(−1) and 960.9 mL·g^(−1)·min^(−1) H_(2) during the first minute of the hydrolysis,respectively.In addition,the MgCl_(2) solution allows repeated use by filtering and exhibits high cycle stability(20 cycles),therefore leading to much reduced capacity loss caused by the excess H_(2)O.We show that by introducing B_(2)O_(3) and recycling the 0.5 M MgCl_(2) solution,the system hydrogen capacity can approach 5.9 wt%,providing a promising hydrogen generation scheme to supply hydrogen to the fuel cells.
基金National Natural Science Foundation of China,Grant/Award Number:21805166111 Project of China,Grant/Award Number:D20015+1 种基金Ministryof Education,Hubei province,China,Grant/Award Number:T2020004Foundation of Science and Technology Bureau of Yichang City,Grant/Award Number:A21‐3‐012。
文摘In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts Pd/carbon nanosphere(CNS),obtained via immobilization of ultrafine Pd nanoparticles onto CNS,are developed and employed for both selective H_(2)generation from HCOOH dehydrogenation and O_(2)evolution from H_(2)O_(2)decomposition.In these reactions,the highest activities for Pd/CNS-800(i.e.,calcinated at 800℃)are 2478 h−1 and 993 min^(−1)for H_(2)and O_(2)evolution,respectively.The highly efficient and selective“on-off”switch for selective H_(2)generation from HCOOH is successfully realized by pH adjustment.This novel and highly efficient nanocatalyst Pd/CNS-800 not only provides new approaches for the promising application of HCOOH and H_(2)O_(2)as economic and safe H_(2)and O_(2)carriers,respectively,for fuel cells,but also promotes the development of“on-off”switch for on-demand H_(2)evolution.
基金Projects(51571112,51171079,51471087) supported by the National Natural Science Foundation of ChinaProject(13KJA430003) supported by Jiangsu Higher Education Institutions of China+1 种基金Project supported by Qing Lan Project,ChinaProject supported by the Priority Academic Program Development(PAPD) of Jiangsu Higher Education Institutions,China
文摘The effects of chloride salts(NaCl,MgCl2and NH4Cl)on the hydrolysis kinetics of MgH2prepared by hydridingcombustion synthesis and mechanical milling(HCS+MM)were discussed.X-ray diffraction(XRD)analyses show that high-purityMgH2was successfully prepared by HCS.Hydrolysis performance test results indicate that the chloride salt added during the millingprocess is favorable to the initial reaction rate and hydrogen generation yield within60min.A MgH2?10%NH4Cl composite exhibitsthe best performance with the hydrogen generation yield of1311mL/g and a conversion rate of85.69%in60min at roomtemperature.It is suggested that the chloride salts not only play as grinding aids in the milling process,but also create fresh surface ofreactive materials,favoring the hydrolysis reaction.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.51704188,51702199,61705125,51802181)the State Key Laboratory of Solidification Processing in NWPU(Grant No.SKLSP201809)+2 种基金Natural Science Foundation of Shaanxi Province(Grant No.2019JQ-099)Research Starting Foundation from Shaanxi University of Science and Technology(Grant No.2016GBJ-04)the financial support of China Scholarship Council(Grant No.201808610089)。
文摘In this work,La-doped Mg-Ni multiphase alloys were prepared by resistance melting furnace(RMF)and then modified by high-energy ball milling(HEBM).The hydrolysis H_(2) generation kinetics/thermodynamics of prepared alloys in Na Cl solutions have been investigated with the help of nonlinear and linear fitting by Avrami-Erofeev and Arrhenius equations.Combining the microstructure information before and after hydrolysis and thermodynamics fitting results,the hydrolysis H_(2) generation mechanism based on nucleation&growth has been elaborated.The final H_(2) generation capacities of 0La,5La,10La and 15 La alloys are 677,653,641 and 770 m L·g^(-1)H_(2) in 240 min at291 K,respectively.While,the final H_(2) generation capacities of HEBM 0La,5La,10La and 15 La alloys are 632,824,611 and 653 m L·g^(-1)H_(2) in 20 min at 291 K,respectively.The as-cast 15La alloy and HEMB 5La alloy present the best H_(2) production rates and final H_(2) production capacities,especially the HEBM 5La can rapidly achieve high H_(2) generation capacity(670 and 824 m L·g^(-1)H_(2) )at low temperature(291 K)within short time(5 and 20 min).The difference between the H_(2) generation capacities is mainly originated from the initial nucleation rate of Mg(OH)_(2) and the subsequent processes affected by the microstructures and phase compositions of the hydrolysis alloys.Relative low initial nucleation rate and fully growth of Mg(OH)_(2) nucleus are the premise of high H_(2) generation capacity due to the hydrolysis H_(2) generation process consisted by the nucleation,growth and contacting of Mg(OH)_(2) nucleus.To utilization H_(2) by designing solid state H_(2) generators using optimized Mg-based alloys is expected to be a feasible H_(2) generation strategy at the moment.
基金supported by Shanxi Province Science Foundation (20210302124446202102070301018)+1 种基金the National Natural Science Joint Foundation (U1710112)Basic Research Project from the Institute of Coal Chemistry, CAS (SCJC-HN-2022-17)。
文摘Hydrogen peroxide(H_(2)O_(2)) is a high-demand organic chemical reagent and has been widely used in various modern industrial applications. Currently,the prominent method for the preparation of H_(2)O_(2) is the anthraquinone oxidation.Unfortunately, it is not conducive to economic and sustainable development since it is a complex process and involves unfriendly environment and potential hazards. In this context, numerous approaches have been developed to synthesize H_(2)O_(2). Among them, photo/electro-catalytic ones are considered as two of the most promising manners for on-site synthesis of H_(2)O_(2). These alternatives are sustainable in that only water or O_(2) is required. Namely, water oxidation(WOR) or oxygen reduction(ORR)reactions can be further coupled with clean and sustainable energy. For photo/electro-catalytic reactions for H_(2)O_(2) generation, the design of the catalysts is extremely important and has been extensively conducted with an aim to obtain ultimate catalytic performance. This article overviews the basic principles of WOR and ORR,followed by the summary of recent progresses and achievements on the design and performance of various photo/electro-catalysts for H_(2)O_(2) generation. The related mechanisms for these approaches are highlighted from theoretical and experimental aspects. Scientific challenges and opportunities of engineering photo/electro-catalysts for H_(2)O_(2) generation are also outlined and discussed.
基金supported by the“National Natural Science Foundation of China (Nos.51902162,21901154)”the FoundationResearch Project of Jiangsu Province (BK20221338)+1 种基金Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources,International Innovation Center for Forest Chemicals and Materials,Nanjing Forestry University,merit-based funding for Nanjing innovation and technology projects,Shanghai Pujiang Program (21PJD022)the Foundation of Jiangsu Key Lab of Biomass Energy and Material (JSBEM-S-202101).
文摘Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous carbon materials composed of abundant graphene/hexagonal boron nitride(G/h-BN)heterostructures.Metal Ni powder and nanoscale h-BN sheets are used as a catalytic substrate/hard template and“nucleation seed”for the formation of the heterostructure,respectively.As-prepared G/h-BN heterostructures exhibit enhanced electrocatalytic activity toward H_(2)O_(2) generation with 86%-95%selectivity at the range of 0.45-0.75 V versus reversible hydrogen electrode(RHE)and a positive onset potential of 0.79 versus RHE(defined at a ring current density of 0.3 mA cm^(-2))in the alkaline solution.In a flow cell,G/h-BN heterostructured electrocatalyst has a H_(2)O_(2) production rate of up to 762 mmol g_(catalyst)^(-1) h^(-1) and Faradaic efficiency of over 75%during 12 h testing,superior to the reported carbon-based electrocatalysts.The density functional theory simulation suggests that the B atoms at the interface of the G/h-BN heterostructure are the key active sites.This research provides a new route to activate carbon catalysts toward highly active and selective O_(2)-to-H_(2)O_(2) conversion.
