摘要：Efficient photogenerated carrier migration/separation plays a critical role in increasing the photocatalytic performance of g-C_(3)N_(4).Herein,sulfonic acid group-functionalized g-C_(3)N_(4)(SACN)was synthesized and then synchronously strengthened by a facile-solid-state thermal reaction of g-C_(3)N_(4)and sulfamic *** a solid strong acid,sulfamic acid can be used to achieve acid etching on the surface of g-C_(3)N_(4)with the assistance of thermal treatment,leading to an enlarged specific surface area and increased surface catalytic reaction *** importantly,our experiments and density functional theory calculations indicate that the driving force generated by the negative inductive effect of sulfonic acid groups significantly improves the charge transfer dynamics and effectively inhibits their ***,the negative inductive effect can induce charge redistribution,which reduces the conduction band potential of g-C_(3)N_(4)to enhance the reduction ability of photo-induced *** a result,the SACN-400 sample showed excellent photocatalytic performance in H2 generation with an apparent quantum efficiency of 11.03%at 420±15 nm,as well as an efficient photodegradation rate for organic pollutants.

摘要：Z-scheme photocatalytic system has been regarded as a popular field of research in photoelectrochemical(PEC)water *** the many obstacles facing a Z-scheme photocatalytic system,the analysis methods of interfacial Z-scheme charge transfer still remain a significant ***,in this study,CdS/Ti-Fe_(2)O_(3)heterojunction photoanodes are elaborately designed to explore the charge-transfer behavior in PEC water *** this study,photophysical measurements,including the Kelvin probe measurement,surface photovoltage spectroscopy(SPV),and transient photovoltage spectroscopy(TPV),are used to monitor the migration behavior of photogenerated charges at the interface electric field of CdS/Ti-Fe_(2)O_(3)Z-scheme heterojunction *** Kelvin probe and SPV measurements demonstrate that CdS/Ti-Fe_(2)O_(3)interfacial driving force favors the rapid transfer of photoexcited electrons to *** double-beam strategy based on TPV indicates that more electrons of Ti-Fe_(2)O_(3)are combined with the holes of CdS owing to the intensive interface electric *** results of these measurements successfully prove the Z-scheme migration mechanism of CdS/Ti-Fe_(2)O_(3)*** from the desirable charge transfer at the interface electric field,CdS/Ti-Fe_(2)O_(3)photoanodes exhibit superior photocatalytic oxygen evolution reaction performance compared with that of pure Ti-Fe_(2)O_(3).The photocurrent density of the 25CdS/Ti-Fe_(2)O_(3)photoanode reaches 1.94 mA/cm^(2) at 1.23 V versus reversible hydrogen electrode without excess cocatalyst,and it is two times higher than that of pure Ti-Fe_(2)O_(3)***,an outstanding strategy is provided in this study to prove the Z-scheme charge-transfer mechanism of photocatalytic systems in PEC water splitting.

摘要：Rational composition design of trimetallic phosphide catalysts is of significant importance for enhanced surface reaction and efficient catalytic ***,hierarchical Co_(x)Ni_(y)Fe_(z)P with precise control of stoichiometric metallic elements(x:y:z=(1-10):(1-10):1)has been synthesized,and Co_(1.3)Ni_(0.5)Fe_(0.2)P,as the most optimal composition,exhibits remarkable catalytic activity(η=320 mV at 10 mA cm^(−2))and long-term stability(ignorable decrease after 10 h continuous test at the current density of 10 mA cm^(−2))toward oxygen evolution reaction(OER).It is found that the surface P in Co_(1.3)Ni_(0.5)Fe_(0.2)P was replaced by O under the OER *** density function theory calculations before and after long-term stability tests suggest the clear increasing of the density of states near the Fermi level of Co_(1.3)Ni_(0.5)Fe_(0.2)P/Co_(1.3)Ni_(0.5)Fe_(0.2)O,which could enhance the OH−adsorption of our electrocatalysts and the corresponding OER performance.

摘要：Rapid industrialization has accordingly increased the demand for *** has resulted in the increasingly severe energy and environmental *** production,based on the photocatalytic water splitting driven by sunlight,is able to directly convert solar energy into a usable or storable energy resource,which is considered to be an ideal alternative energy source to assist in solving the energy crisis and environmental ***,the hydrogen production efficiency of single phase photocatalysts is too low to meet the practical *** construction of heterostructured photocatalyst systems,which are comprised of multiple components or multiple phases,is an efficient method to facilitate the separation of electron‐hole pairs to minimize the energy‐waste,provide more electrons,enhance their redox ability,and hence improve the photocatalytic *** summarize the recent progress in the rational design and fabrication of nanoheterostructured *** heterojunction photocatalytic hydrogen generation systems can be divided into type‐I,type‐II,pn‐junction and Z‐scheme junction,according to the differences in the transfer of the photogenerated electrons and ***,a summary and some of the challenges and prospects for the future development of heterojunction photocatalytic systems are discussed.

摘要：Nonprecious metal-based oxygen reduction reaction(ORR)electrocatalysts with high efficiency in both alkaline and acidic media are being intensively studied for the purpose of replacing expensive Pt-based catalysts;however,it is still a challenge to achieve superior ORR performances,especially in acidic ***,by pyrolysis of mixed precursors of diammonium phosphate,melamine and hemin,we prepared a nanocomposite catalyst(denoted as FeP@PGL)composed of nitrogen-doped carbon nanosheets with embedded FeP nanoparticles(NPs),which were encapsulated by in-situ formed phosphorus-doped graphene *** is found that phosphorous was preferentially doped in the coating layers on FeP NPs,instead of in the carbon *** FeP@PGL catalyst exhibited excellent ORR performance,with the onset and half-wave potential up to 1.01 and 0.90 V *** reversible hydrogen electrode(RHE)in alkaline media,and0.95 and 0.81 V *** in acidic media,*** thorough microscopy and spectroscopy characterizations,the interfacial charge transfer between the encapsulated FeP NPs and P-doped graphene layers was identified,and the local work function of the catalyst surface was also reduced by the interfacial *** interfacial synergy between the encapsulated FeP and phosphorus-doped graphene layers was essential to enhance the ORR *** study not only demonstrates the promising ORR properties of the encapsulated-FeP-based nanocomposite catalyst,but also provides direct evidence of the interfacial charge transfer effect and its role in ORR process.

摘要：Obtaining a detailed understanding of the surface modification of supports is crucial;however,it is a challenging task for the development and large-scale fabrication of supported electrocatalysts that can be used as alternatives to Pt-based catalysts for the oxygen reduction reaction(ORR).In this study,commercial silicon carbide(SiC)was modified through surface oxidization(O-SiC)to support the use of Pd nanoparticles(Pd NPs)as electrocatalysts for *** obtained Pd/O-SiC catalysts exhibited better ORR activity,stronger durability,and higher resistance to methanol poisoning than that exhibited by commercial Pt/*** role of the support in enhancing the ORR performance,especially the oxidization of SiC surfaces,was discussed in detail based on the experimental characterizations and density functional theory *** underlying mechanism of the superior ORR performance of Pd/O-SiC catalysts was attributed to the charge transfer from SiC_(x)O_(y)to Pd NPs on the surfaces of SiC and the strong metal–support interactions(SMSIs)between Pd and SiC_(x)O_(y).The charge transfer enhanced the ORR activity by inducing electron-rich Pd,increased the adsorption of the key intermediate OOH,and decreased the Gibbs free energy of the critical ORR ***,SMSIs enhanced the ORR stability of the Pd/O-SiC *** study provided a facile route for designing and developing highly active Pd-based ORR electrocatalysts.

摘要：Although CO_(2)photoreduction is a promising method for solar‐to‐fuel conversion,it suffers from low charge transfer efficiency of the *** improve the CO_(2)photoreduction performance,introduction of electron‐accumulated materials on the photocatalyst surface is considered an effective *** this study,the Bi_(19)S_(27)Br_(3)/BiOBr composites were designed and *** Bi19S27Br3 nanorod in this photocatalytic system acts as an electron‐accumulated active site for extracting the photogenerated electrons on the BiOBr surface and for effectively activating the CO2 *** a result,Bi_(19)S_(27)Br_(3)/BiOBr composites exhibit the higher charge carrier transfer efficiency and further improves the CO_(2)photoreduction performance relative to that of pure Bi_(19)S_(27)Br_(3)and *** rate of CO formation using Bi_(19)S_(27)Br_(3)/BiOBr‐5 is about 8.74 and 2.40 times that using Bi_(19)S_(27)Br_(3)and BiOBr,*** work provides new insights for the application of Bi_(19)S_(27)Br_(3)as an electron‐accumulating site for achieving high photocatalytic CO2 reduction performance in the future.