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Embedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting
A robust and efficient dye-sensitized NiO bio-hybrid photocathode based on a redox polymer and [FeFe]- hydrogenase has been developed to couple with a BiVO4 photoanode for water splitting without applied bias.
- Fangwen Cheng
- , Olha Pavliuk
- & Haining Tian
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| Open Access
Induced dipole moments in amorphous ZnCdS catalysts facilitate photocatalytic H2 evolution
The rapid recombination of photogenerated charge carriers is a key challenge for photocatalytic hydrogen production. Here, the authors report an amorphous ZnCdS to break the symmetry of atom arrangement that induces strong dipole fields, thus providing extra driving forces for charge separation.
- Xin Wang
- , Boyan Liu
- & Songcan Wang
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Stable water splitting using photoelectrodes with a cryogelated overlayer
Photoelectrodes made of earth-abundant materials can contribute to low-cost and carbon-free hydrogen production, but suffer from a short lifetime. Here the authors report cryogel overlayer to increase the operation time of the device by regulating evolving hydrogen bubble dynamics.
- Byungjun Kang
- , Jeiwan Tan
- & Hyungsuk Lee
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| Open Access
Decoupled electrolysis for hydrogen production and hydrazine oxidation via high-capacity and stable pre-protonated vanadium hexacyanoferrate
Decoupled electrolysis with the aid of a redox mediator offers great flexibility in operation. Here, the authors construct a decoupled electrolysis system for separate hydrogen production and electricity generation to achieve flexible energy conversion and storage using renewables.
- Fei Lv
- , Jiazhe Wu
- & Yubin Chen
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Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure
Designing an organic polymer photocatalyst for efficient hydrogen evolution in the near-infrared (NIR) light region is still a major challenge. The authors present here a series of polymer nanoparticles for a efficient hydrogen evolution under visible and NIR light irradiation, without combining or hybridizing with other materials.
- Mohamed Hammad Elsayed
- , Mohamed Abdellah
- & Ho-Hsiu Chou
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Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system
Direct participation of plasmon-induced hot electrons in the photoelectrocatalytic synthesis of hydrogen. This report solves a long-lasting contentious issue surrounding plasmonic materials on catalytic applications.
- Ananta Dey
- , Amal Mendalz
- & Jacinto Sá
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Operando formation of highly efficient electrocatalysts induced by heteroatom leaching
Stability of catalyst dopant species under working conditions is often unexplored. Here, the authors reveal that the dopant sites tend to collapse when the applied potential is too negative or too positive and describe a protocol for the in-situ formation of highly efficient active sites via the leaching of dopants.
- Cong Liu
- , Bingbao Mei
- & Weilin Xu
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Green electrosynthesis of 3,3’-diamino-4,4’-azofurazan energetic materials coupled with energy-efficient hydrogen production over Pt-based catalysts
The hybrid water electrolysis system enables a potential for high-efficiency H2 production. Here, the authors propose an electrosynthesis of azo-energetic material coupled with water electrolysis, realizing energy-saving H2 production and obtaining azo-energetic materials via a green pathway.
- Jiachen Li
- , Yuqiang Ma
- & Jieshan Qiu
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Stabilizing ruthenium dioxide with cation-anchored sulfate for durable oxygen evolution in proton-exchange membrane water electrolyzers
Designing stable Ru-based catalysts for acidic oxygen evolution remains a challenge. Here, the authors propose an oxyanion protection strategy to prevent the formation of oxygen vacancies on the RuO2 surface by creating coordination-saturated lattice oxygen, thereby greatly enhancing the stability.
- Yanrong Xue
- , Jiwu Zhao
- & Xu Lu
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Single-crystal ZrCo nanoparticle for advanced hydrogen and H-isotope storage
ZrCo, a promising hydrogen isotope storage material, has poor cyclic storage capacity. Here author reveal a defect-derived disproportionation mechanism and report a nano-single-crystal strategy to comprehensively improve performances.
- Zhenyang Li
- , Shiyuan Liu
- & Jianglan Shui
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| Open Access
Corrosion-resistant cobalt phosphide electrocatalysts for salinity tolerance hydrogen evolution
Seawater electrolysis for hydrogen production is limited by the poor salinity tolerance of catalysts. CoP was found to repel chlorine while attracting H2O molecules to form a thin layer on the catalyst surface, thus constructing a corrosion-resistant CoP/rGO@Ti catalyst for seawater splitting.
- Xinwu Xu
- , Yang Lu
- & Yibo He
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| Open Access
Synergistic effects of mixing and strain in high entropy spinel oxides for oxygen evolution reaction
Efficient and durable electrocatalysts are essential for boosting oxygen evolution reaction toward hydrogen production. Here, the authors report a combined theoretical and experimental study on high-entropy spinel oxide with element mixing and strains providing superior activity and stability.
- Jihyun Baek
- , Md Delowar Hossain
- & Xiaolin Zheng
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Reliable bi-functional nickel-phosphate /TiO2 integration enables stable n-GaAs photoanode for water oxidation under alkaline condition
Photocorrosion limits the efficiency and stability of gallium arsenide photoanodes. Here the authors report crystalline TiO2 passivation with Ni-phosphate hole-sink layer which enables rapid charge transport for enhanced photostability of 110 h.
- Maheswari Arunachalam
- , Rohini Subhash Kanase
- & Soon Hyung Kang
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Efficient and sustainable water electrolysis achieved by excess electron reservoir enabling charge replenishment to catalysts
Charge replenishment from the supports to catalysts can play a key role in stabilizing active-Ir(III) to realize an efficient and durable oxygen evolution reaction. Here, the authors report an excess electron reservoir, greatly enhancing charge donation for improved water-splitting performance.
- Gyu Rac Lee
- , Jun Kim
- & Yeon Sik Jung
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Turing structuring with multiple nanotwins to engineer efficient and stable catalysts for hydrogen evolution reaction
Developing new electrocatalysts for hydrogen production is of high interests. Here the authors report PtNiNb with high-density nanotwins and large strain as hydrogen evolution catalysts in anion-exchange-membrane water electrolyser.
- Jialun Gu
- , Lanxi Li
- & Jian Lu
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Ionomer-free and recyclable porous-transport electrode for high-performing proton-exchange-membrane water electrolysis
The supply of iridium is likely to become a bottleneck for hydrogen production. Here, authors develop ionomer-free porous transport electrodes with low iridium loading designed to improve manufacturability and recyclability of electrodes for proton exchange membrane water electrolyzers.
- Jason K. Lee
- , Grace Anderson
- & Xiong Peng
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| Open Access
Tailoring a local acid-like microenvironment for efficient neutral hydrogen evolution
The development of neutral hydrogen evolution catalysts is challenging due to their sluggish kinetics. Here the authors report HxWO3 support which acts as proton sponge to create a local acid-like microenvironment around Ir sites, realizing acid-like hydrogen evolution rate in neutral media.
- Xiaozhong Zheng
- , Xiaoyun Shi
- & Yong Wang
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A sodium-ion-conducted asymmetric electrolyzer to lower the operation voltage for direct seawater electrolysis
Hydrogen produced directly from neutral seawater is promising but challenging due to seawater’s complex composition. Here, the authors report a Na+-conducted pH-asymmetric electrolyzer that can directly split seawater into hydrogen with low electricity cost and nearly zero chloride interference.
- Hao Shi
- , Tanyuan Wang
- & Qing Li
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Integrated halide perovskite photoelectrochemical cells with solar-driven water-splitting efficiency of 20.8%
High-efficiency photoelectrodes, which integrate light absorption with catalysis, have been limited to costly materials. Here, the authors develop an anticorrosion barrier that enables low-cost semiconductors for integrated solar fuel devices with 20.8% solar-to-hydrogen energy conversion efficiency.
- Austin M. K. Fehr
- , Ayush Agrawal
- & Aditya D. Mohite
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Carbon neutral hydrogen storage and release cycles based on dual-functional roles of formamides
The search for new carbon-based hydrogen storage materials attracts scientists from various disciplines. Now, carbon-neutral hydrogen storage-release is reported based on dual-functional roles of formamides and uses non-noble, Fe-based catalyst.
- Duo Wei
- , Xinzhe Shi
- & Matthias Beller
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Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics
Photocatalytic hydrogen evolution efficiency is limited due to unfavorable carrier dynamics and thermodynamic performance. Here, the authors report an electric double-layer-mediated polarization field to improve carrier dynamics and optimize the thermodynamics by regulating the coordination of surface atoms.
- Chengxin Zhou
- , Jian Gao
- & Chuan Xia
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Global green hydrogen-based steel opportunities surrounding high quality renewable energy and iron ore deposits
Facility-level analysis of green H2- based steel production demonstrates co-location of high-quality renewables and iron ore resources is imperative for cost minimisation.
- Alexandra Devlin
- , Jannik Kossen
- & Aidong Yang
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Bioelectrocatalysis with a palladium membrane reactor
Enzymatic catalysis requires cofactors such as NAD(P)H, whose regeneration is currently accomplished via secondary enzymes or electrolytic cell. Here, the authors report an electrochemical method of cofactors regeneration without supporting enzymes or mediators, nor formation of NAD2 dimers.
- Aiko Kurimoto
- , Seyed A. Nasseri
- & Curtis P. Berlinguette
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An electron-hole rich dual-site nickel catalyst for efficient photocatalytic overall water splitting
Vast majority of photocatalysts for hydrogen production relies on additional sacrificial agents and noble metal cocatalysts. It is of great importance yet challenging to achieve photocatalytic overall water splitting with decent performance. Here, the authors report Ni2P based photocatalyst assisted by H2O2-craking reaction for overall water splitting with H2 and O2 production of 1507 μmol h−1 g−1 H2 and 702 μmol h−1 g−1.
- Xiaoqing Yan
- , Mengyang Xia
- & Guidong Yang
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Unraveling a bifunctional mechanism for methanol-to-formate electro-oxidation on nickel-based hydroxides
Understanding the active sites is essential for advanced catalyst design. Here, the authors report a bifunctional mechanism for the methanol electrooxidation reaction using NiMn hydroxide with NiIII and oxygen active sites which work in a cooperative manner to promote either spontaneous or non-spontaneous methanol oxidation.
- Botao Zhu
- , Bo Dong
- & Lai Feng
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Diversity of platinum-sites at platinum/fullerene interface accelerates alkaline hydrogen evolution
One major technological obstacle for membrane-based alkaline water electrolyzer is the inefficient hydrogen evolution reaction. Here, the authors report a platinum/fullerene heterostructure catalyst, which shows enhanced activity for hydrogen production due to the diverse interface between platinum and fullerene.
- Jiayi Chen
- , Mohammed Aliasgar
- & Lei Wang
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Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation
Exploring highly active and durable Ru-based electrocatalysts for acidic water oxidation is challenging. Here authors reported an ion-exchange adsorption strategy to regulate oxygen vacancies and Rh dopant, with a corresponding fundamental investigation on the lattice oxygen oxidation and the oxygen vacancy site.
- Yi Wang
- , Rong Yang
- & Zhong-Shuai Wu
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Life cycle net energy assessment of sustainable H2 production and hydrogenation of chemicals in a coupled photoelectrochemical device
Integrating green hydrogen production with the generation of valuable chemicals has the potential to increase the competitiveness of the system. Here, the authors quantitatively evaluate the energetic benefit of coupling hydrogen production with the hydrogenation of feedstocks in a photoelectrochemical device.
- Xinyi Zhang
- , Michael Schwarze
- & Fatwa F. Abdi
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Integrated interfacial design of covalent organic framework photocatalysts to promote hydrogen evolution from water
Attempts to develop hydrogen evolution photocatalysts usually result in low efficiency. Here the authors report a photocatalyst system by integrated interfacial design of stable covalent organic frameworks for high performance hydrogen evolution.
- Ting He
- , Wenlong Zhen
- & Donglin Jiang
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Oriented intergrowth of the catalyst layer in membrane electrode assembly for alkaline water electrolysis
While membrane electrode assembly water electrolyzers are a promising renewable energy technology, further optimizations are needed before wide-spread implementation can occur. Here, authors examine a device with a porous membrane that enables oriented catalyst intergrowth to improve performances.
- Lei Wan
- , Maobin Pang
- & Baoguo Wang
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Observation of a robust and active catalyst for hydrogen evolution under high current densities
The development of robust catalysts that could work under industrial-scale current densities is a challenge for hydrogen production. Here, the authors report an in-situ activation method to produce ferromagnetic Ru clusters that can catalyze the hydrogen evolution reaction at high current densities.
- Yudi Zhang
- , Kathryn E. Arpino
- & Guowei Li
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Risk of the hydrogen economy for atmospheric methane
H2 has the potential to become the green, low-carbon fuel of the future. However, hydrogen emissions impact atmospheric methane (CH4). Bertagni et al. investigate the fate of atmospheric CH4 in scenarios of H2 economy.
- Matteo B. Bertagni
- , Stephen W. Pacala
- & Amilcare Porporato
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Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide
Hydrogen peroxide production from water electrochemical oxidation is a challenging process. Here the authors report discovery of LaAlO3 after screening a series of perovskites as active, stable, and selective catalyst for electrochemical H2O2 production from water oxidation.
- Jihyun Baek
- , Qiu Jin
- & Xiaolin Zheng
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Accelerated pyro-catalytic hydrogen production enabled by plasmonic local heating of Au on pyroelectric BaTiO3 nanoparticles
While pyrocatalysis offers a means to store energy in chemical bonds from temperature changes, most materials show low conversion efficiencies. Here, authors examine Au nanoparticles on BaTiO3 and demonstrate localized plasmonic heat sources to enhance pyrocatalytic H2 evolution.
- Huilin You
- , Siqi Li
- & Haitao Huang
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Bias-free solar hydrogen production at 19.8 mA cm−2 using perovskite photocathode and lignocellulosic biomass
While light-driven water splitting offers a means to produce renewable H2 fuel, water oxidation limits performances and yields low-value products. Here, authors demonstrate a photoelectrochemical cell that converts lignocellulosic biomass into valuable products alongside H2.
- Yuri Choi
- , Rashmi Mehrotra
- & Jungki Ryu
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The effect of enantioselective chiral covalent organic frameworks and cysteine sacrificial donors on photocatalytic hydrogen evolution
Chiral covalent organic frameworks are demonstrated to enable the docking of sacrificial electron donors via enantioselective combination, thereby improving oxidative half-reaction kinetics and boosting visible photocatalytic H2 production.
- Weijun Weng
- & Jia Guo
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Hydrogen-substituted graphdiyne encapsulated cuprous oxide photocathode for efficient and stable photoelectrochemical water reduction
Cu2O-based photocathodes for photoelectrochemical water reduction suffer severe self-photo-corrosion issue. Here the authors report an in-situ encapsulation strategy with hydrogen-substituted graphdiyne to protect Cu2O for water reduction with a photocurrent density of −12.88 mA cm-2.
- Xue Zhou
- , Baihe Fu
- & Zhonghai Zhang
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| Open Access
Sustainable production of hydrogen with high purity from methanol and water at low temperatures
Carbon neutrality initiative has stimulated the development of the sustainable methodologies for hydrogen generation and safe storage. Here the authors demonstrate that the dual-active sites of Pt single-atoms and frustrated Lewis pairs on porous nanorods of CeO2 enable the efficient additive-free H2 generation with a low CO generation through reforming of methanol and water.
- Sai Zhang
- , Yuxuan Liu
- & Yongquan Qu
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| Open Access
OH spectator at IrMo intermetallic narrowing activity gap between alkaline and acidic hydrogen evolution reaction
While alkaline water electrolysis offers a green means for hydrogen production, H2-evolving catalysts typically show worse activities in alkaline media than in acid. Here, authors examine IrMo intermetallics as electrocatalysts and identify a stably-adsorbed OH spectator in promoting performances.
- Jiaxi Zhang
- , Longhai Zhang
- & Zhiming Cui
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| Open Access
Main-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution
The introduction of hydrophilic segments into the main-chain of polymer photocatalysts allows water to efficiently enter the interior through these hydrophilic segments, and results in effective water/polymer interfaces for hydrogen evolution.
- Chih-Li Chang
- , Wei-Cheng Lin
- & Ho-Hsiu Chou
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Article
| Open Access
Hydrogen production from the air
While obtaining H2 from water splitting offers a promising strategy for renewable fuel production, current technologies rely on liquid freshwater. Here, authors use a hygroscopic electrolyte to achieve electrocatalytic water vapor splitting driven by renewable resources without liquid water.
- Jining Guo
- , Yuecheng Zhang
- & Gang Kevin Li
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| Open Access
Electrocatalytic synthesis of adipic acid coupled with H2 production enhanced by a ligand modification strategy
Adipic acid is an important building block of polymers, although its production relies on harmful reagents. Here, authors examined surfactant-modified nickel hydroxide for adipic acid electrosynthesis coupled with hydrogen gas evolution.
- Zhenhua Li
- , Xiaofan Li
- & Haohong Duan
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Article
| Open Access
Insights into the activity of nickel boride/nickel heterostructures for efficient methanol electrooxidation
Understanding the role of active sites in electrooxidation reactions is important yet challenging. Here, the authors use operando spectroscopies to monitor the effect of methanol concentration on Ni3B/Ni heterostructures during formate production.
- Yanbin Qi
- , Yue Zhang
- & Chunzhong Li
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| Open Access
Bixbyite-type Ln2O3 as promoters of metallic Ni for alkaline electrocatalytic hydrogen evolution
While renewable H2 evolution will require inexpensive, abundant catalysts, non-noble metals typically show relatively low activities. Here, authors examine lanthanide metal sesquioxide doped metallic Ni and show efficient, stable performances for alkaline H2 evolution electrocatalysis.
- Hongming Sun
- , Zhenhua Yan
- & Miao Du
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| Open Access
RuO2 electronic structure and lattice strain dual engineering for enhanced acidic oxygen evolution reaction performance
While water splitting in acid offers higher operational performances than in alkaline conditions, there are few high-activity, acid-stable oxygen evolution electrocatalysts. Here, authors examine electrochemical Li intercalation to improve the activity and stability of RuO2 for acidic water oxidation.
- Yin Qin
- , Tingting Yu
- & Tong-Yi Zhang
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| Open Access
Boosting the performance of single-atom catalysts via external electric field polarization
While single-atom catalysts offer high atomic utilization and tunable reaction pathways, there are still challenges in controlling reactivity. Here, authors use oriented external electric fields to induce electrostatic polarization in metal single-atoms and to boost water-splitting performances.
- Yanghang Pan
- , Xinzhu Wang
- & Mengning Ding
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| Open Access
Modulating Pt-O-Pt atomic clusters with isolated cobalt atoms for enhanced hydrogen evolution catalysis
Modulating single-metal sites at the atomic level can boost the intrinsic catalytic activity. Here, the authors describe the design of Pt atomic clusters containing Pt-O-Pt units supported on Co single atoms and N co-doped carbon for enhanced hydrogen evolution catalysis.
- Yufei Zhao
- , Priyank V. Kumar
- & Xunyu Lu
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| Open Access
Efficient and stable noble-metal-free catalyst for acidic water oxidation
While acidic water splitting offers a renewable means to obtain renewable hydrogen fuel, the catalysts needed to oxidize water often require expensive noble metals. Here, authors show manganese oxyhalides as acidic oxygen evolution electrocatalysts.
- Sanjiang Pan
- , Hao Li
- & Xiaodan Zhang
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| Open Access
A high-performance capillary-fed electrolysis cell promises more cost-competitive renewable hydrogen
Water electrolysis offers a promising means for green hydrogen production, however current electrolysers do not provide a competitive edge over fossil fuels. Here, authors develop a capillary-fed electrolyser setup that avoids bubble formation to achieve a high-performance, cost-competitive device.
- Aaron Hodges
- , Anh Linh Hoang
- & Gordon G. Wallace
Highly efficient anion exchange membrane water electrolyzers via chromium-doped amorphous electrocatalysts