The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past...The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past decades,researchers have reported a number of hydrogen evolution reaction(HER)electrocatalysts with activity comparable to that of commercial Pt/C,but most of them are tested within a small current density range,typically no more than 500 mA cm^(-2).To realize the industrial application of hydrogen production from water electrolysis,it is essential to develop high-efficiency HER electrocatalysts at high current density(HCD≥500 mA cm^(-2)).Nevertheless,it remains challenging and significant to rational design HCD electrocatalysts for HER.In this paper,the design strategy of HCD electrocatalysts is discussed,and some HCD electrocatalysts for HER are reviewed in seven categories(alloy,metal oxide,metal hydroxide,metal sulfide/selenide,metal nitride,metal phosphide and other derived electrocatalysts).At the end of this article,we also pro-pose some viewpoints and prospects for the future development and research directions of HCD electrocatalysts for HER.展开更多
A facile colloidal route to synthesize MoSe2 porous microspheres with diameters of 400-600 nm made up of MoSe2 monolayer flakes （-0.7 nm in thickness） is reported. The solvents trioctylamine （TOA） and oleylamine ...A facile colloidal route to synthesize MoSe2 porous microspheres with diameters of 400-600 nm made up of MoSe2 monolayer flakes （-0.7 nm in thickness） is reported. The solvents trioctylamine （TOA） and oleylamine （OAM） are found to play important roles in the formation of MoSe2 microspheres, whereby TOA determines the three-dimensional （3D） microspherical morphology and OAM directs the formation of MoSes monolayer flakes. The robust 3D MoSe2 microspheres exhibit remarkable activity and durability for the electrocatalytic hydrogen evolution reaction （HER） in acid, maintaining a small onset overpotential of -77 mV and keeping a small overpotential of 100 mV for a current density of 5 mA/cm2 after 1,000 cycles. In addition, similar 3D WSe2 microspheres can also be prepared by using this method. We expect this facile colloidal route could further be expanded to synthesize other porous structures which will find applications in fields such as in energy storage, catalysis, and sensing.展开更多
A low-cost,highly efficient and strong durable bifunctional electrocatalyst is crucial for electrochemical overall water splitting.In this paper,a self-templated strategy combined with in-situ phosphorization is appli...A low-cost,highly efficient and strong durable bifunctional electrocatalyst is crucial for electrochemical overall water splitting.In this paper,a self-templated strategy combined with in-situ phosphorization is applied to construct hollow structured bimetallic cobalt-nickel phosphide(CoNiP_(x))nanocages.Owing to their unique hollow structure and bimetallic synergistic effects,the as-synthesized CoNiP_(x)hollow nanocages exhibit a high electrocatalytic activity and stability towards hydrogen evolution reaction in all-pH electrolyte and a remarkable electrochemical performance for oxygen evolution reaction in 1.0 mol L^(-1)KOH.Meanwhile,with the bifunctional electrocatalyst in both anode and cathode for overall water splitting,a low voltage of 1.61 V and superior stability are achieved at a current density of 20 mA cm^(-2).展开更多
Developing low-cost and earth-abundant electrocatalysts with high performance for electrochemical water splitting is a challenging issue. Herein, we report a facile and effective way to fabricate three-dimension(3D) o...Developing low-cost and earth-abundant electrocatalysts with high performance for electrochemical water splitting is a challenging issue. Herein, we report a facile and effective way to fabricate three-dimension(3D) ordered mesoporous Co1-xFexP(x=0, 0.25, 0.5, 0.75) electrocatalyst.Benefiting from 3D ordered mesoporous pore channels and composition optimization, the Co0.75Fe0.25 P exhibits excellent electrocatalytic activities with low overpotentials of 270 and 209 mV at 10 mA cm^-2 for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER), respectively, in the alkaline electrolyte along with a durable electrochemical stability. In addition, as both the cathode and anode, the Co0.75Fe0.25P also exhibits superior electrolysis water splitting performance with only an applied voltage of 1.63 V to attain a current density of 10 m A cm^-2 without obvious decay for 18 h,indicating that the Co0.75Fe0.25P is an efficient electrocatalyst for overall water splitting.展开更多
Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless,...Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional(2D) Ru-based snow-like nanosheets with Ru/Ru O2interface(Ru/Ru O2SNSs)via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy(HBE) and hydroxide binding energy(OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO_(2) SNSs display a mass activity of 9.13 A mgRu^(–1) at an overpotential of 50 m V in 0.1 mol L^(–1) KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs(0.14 A mg_(Ru)^(–1)), RuO_(2) SNSs(0.03 A mg_(Ru)^(–1)), and commercial Pt/C(0.43 A mg_(Ru)^(–1)), respectively.Moreover, Ru/RuO_(2) SNSs display improved HER activity with a low overpotential of 20.2 m V for achieving10 m A cm^(-2)in 1 mol L^(–1)KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis.展开更多
Low-cost, highly efficient catalysts for hydrogen evolution reaction(HER) are very important to advance energy economy based on clean hydrogen gas. Intensive studies on two-dimensional molybdenum disulfides(2 D Mo S2)...Low-cost, highly efficient catalysts for hydrogen evolution reaction(HER) are very important to advance energy economy based on clean hydrogen gas. Intensive studies on two-dimensional molybdenum disulfides(2 D Mo S2) have been conducted due to their remarkable catalytic properties.However, most of the reported syntheses are time consuming,complicated and less efficient. The present work demonstrates the production of Mo S2/graphene catalyst via an ultra-fast(60 s) microwave-initiated approach. High specific surface area and conductivity of graphene delivers a favorable conductive network for the growth of Mo S2 nanosheets, along with rapid charge transfer kinetics. As-produced Mo S2/graphene nanocomposites exhibit superior electrocatalytic activity for the HER in acidic medium, with a low onset potential of62 m V, high cathodic currents and a Tafel slope of43.3 m V/decade. Beyond excellent catalytic activity, Mo S2/graphene reveals long cycling stability with a very high cathodic current density of around 1000 m A cm^-2 at an overpotential of 250 m V. Moreover, the Mo S2/graphene-catalyst exhibits outstanding HER activities in a temperature range of 30 to 120°C with low activation energy of36.51 k J mol^-1, providing the opportunity of practical scalable processing.展开更多
文摘The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past decades,researchers have reported a number of hydrogen evolution reaction(HER)electrocatalysts with activity comparable to that of commercial Pt/C,but most of them are tested within a small current density range,typically no more than 500 mA cm^(-2).To realize the industrial application of hydrogen production from water electrolysis,it is essential to develop high-efficiency HER electrocatalysts at high current density(HCD≥500 mA cm^(-2)).Nevertheless,it remains challenging and significant to rational design HCD electrocatalysts for HER.In this paper,the design strategy of HCD electrocatalysts is discussed,and some HCD electrocatalysts for HER are reviewed in seven categories(alloy,metal oxide,metal hydroxide,metal sulfide/selenide,metal nitride,metal phosphide and other derived electrocatalysts).At the end of this article,we also pro-pose some viewpoints and prospects for the future development and research directions of HCD electrocatalysts for HER.
文摘A facile colloidal route to synthesize MoSe2 porous microspheres with diameters of 400-600 nm made up of MoSe2 monolayer flakes （-0.7 nm in thickness） is reported. The solvents trioctylamine （TOA） and oleylamine （OAM） are found to play important roles in the formation of MoSe2 microspheres, whereby TOA determines the three-dimensional （3D） microspherical morphology and OAM directs the formation of MoSes monolayer flakes. The robust 3D MoSe2 microspheres exhibit remarkable activity and durability for the electrocatalytic hydrogen evolution reaction （HER） in acid, maintaining a small onset overpotential of -77 mV and keeping a small overpotential of 100 mV for a current density of 5 mA/cm2 after 1,000 cycles. In addition, similar 3D WSe2 microspheres can also be prepared by using this method. We expect this facile colloidal route could further be expanded to synthesize other porous structures which will find applications in fields such as in energy storage, catalysis, and sensing.
基金the National Key R&D Program of China(2017YFA 0208300 and 0700104)the National Natural Science Foundation of China(21671180)the State Key Laboratory of Organic Inorganic Composites(oic-201801007)。
文摘A low-cost,highly efficient and strong durable bifunctional electrocatalyst is crucial for electrochemical overall water splitting.In this paper,a self-templated strategy combined with in-situ phosphorization is applied to construct hollow structured bimetallic cobalt-nickel phosphide(CoNiP_(x))nanocages.Owing to their unique hollow structure and bimetallic synergistic effects,the as-synthesized CoNiP_(x)hollow nanocages exhibit a high electrocatalytic activity and stability towards hydrogen evolution reaction in all-pH electrolyte and a remarkable electrochemical performance for oxygen evolution reaction in 1.0 mol L^(-1)KOH.Meanwhile,with the bifunctional electrocatalyst in both anode and cathode for overall water splitting,a low voltage of 1.61 V and superior stability are achieved at a current density of 20 mA cm^(-2).
基金supported by the National Natural Science Foundation of China (51571072 and 51871078)Heilongjiang Science Foundation (E2018028)
文摘Developing low-cost and earth-abundant electrocatalysts with high performance for electrochemical water splitting is a challenging issue. Herein, we report a facile and effective way to fabricate three-dimension(3D) ordered mesoporous Co1-xFexP(x=0, 0.25, 0.5, 0.75) electrocatalyst.Benefiting from 3D ordered mesoporous pore channels and composition optimization, the Co0.75Fe0.25 P exhibits excellent electrocatalytic activities with low overpotentials of 270 and 209 mV at 10 mA cm^-2 for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER), respectively, in the alkaline electrolyte along with a durable electrochemical stability. In addition, as both the cathode and anode, the Co0.75Fe0.25P also exhibits superior electrolysis water splitting performance with only an applied voltage of 1.63 V to attain a current density of 10 m A cm^-2 without obvious decay for 18 h,indicating that the Co0.75Fe0.25P is an efficient electrocatalyst for overall water splitting.
基金supported by the National Key R&D Program of China(2020YFB1505802)the Ministry of Science and Technology of China(2017YFA0208200,2016YFA0204100)+4 种基金the National Natural Science Foundation of China(22025108,U21A20327,and22121001)China Postdoctoral Science Foundation(2020M682083)Guangdong Provincial Natural Science Fund for Distinguished Young Scholars(2021B1515020081)Start-up Support from Xiamen University and the Guangzhou Key Laboratory of Low Dimensional Materials and Energy Storage Devices(20195010002)。
文摘Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional(2D) Ru-based snow-like nanosheets with Ru/Ru O2interface(Ru/Ru O2SNSs)via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy(HBE) and hydroxide binding energy(OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO_(2) SNSs display a mass activity of 9.13 A mgRu^(–1) at an overpotential of 50 m V in 0.1 mol L^(–1) KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs(0.14 A mg_(Ru)^(–1)), RuO_(2) SNSs(0.03 A mg_(Ru)^(–1)), and commercial Pt/C(0.43 A mg_(Ru)^(–1)), respectively.Moreover, Ru/RuO_(2) SNSs display improved HER activity with a low overpotential of 20.2 m V for achieving10 m A cm^(-2)in 1 mol L^(–1)KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis.
基金supported by Auburn UniversityIntramural Grants Program (AU-IGP)
文摘Low-cost, highly efficient catalysts for hydrogen evolution reaction(HER) are very important to advance energy economy based on clean hydrogen gas. Intensive studies on two-dimensional molybdenum disulfides(2 D Mo S2) have been conducted due to their remarkable catalytic properties.However, most of the reported syntheses are time consuming,complicated and less efficient. The present work demonstrates the production of Mo S2/graphene catalyst via an ultra-fast(60 s) microwave-initiated approach. High specific surface area and conductivity of graphene delivers a favorable conductive network for the growth of Mo S2 nanosheets, along with rapid charge transfer kinetics. As-produced Mo S2/graphene nanocomposites exhibit superior electrocatalytic activity for the HER in acidic medium, with a low onset potential of62 m V, high cathodic currents and a Tafel slope of43.3 m V/decade. Beyond excellent catalytic activity, Mo S2/graphene reveals long cycling stability with a very high cathodic current density of around 1000 m A cm^-2 at an overpotential of 250 m V. Moreover, the Mo S2/graphene-catalyst exhibits outstanding HER activities in a temperature range of 30 to 120°C with low activation energy of36.51 k J mol^-1, providing the opportunity of practical scalable processing.
