Browse Articles

  • Article |

    Platinum plays a crucial role in various electrocatalytic systems, but its scarcity and cost limit its practical application. Now, a single-atom tailoring strategy applied to platinum nanowires maximizes their specific and mass activities for the hydrogen evolution and methanol and ethanol oxidation reactions.

    • Mufan Li
    • , Kaining Duanmu
    • , Chengzhang Wan
    • , Tao Cheng
    • , Liang Zhang
    • , Sheng Dai
    • , Wenxin Chen
    • , Zipeng Zhao
    • , Peng Li
    • , Huilong Fei
    • , Yuanming Zhu
    • , Rong Yu
    • , Jun Luo
    • , Ketao Zang
    • , Zhaoyang Lin
    • , Mengning Ding
    • , Jin Huang
    • , Hongtao Sun
    • , Jinghua Guo
    • , Xiaoqing Pan
    • , William A. Goddard III
    • , Philippe Sautet
    • , Yu Huang
    •  & Xiangfeng Duan
  • Perspective |

    While converting methane to methanol is an attractive process, making a catalytic—and commercially viable—route has presented severe difficulties. Here van Bokhoven and co-workers discuss the successes, problems and misconceptions in the field, focusing on the reaction with molecular oxygen over zeolites.

    • Manoj Ravi
    • , Vitaly L. Sushkevich
    • , Amy J. Knorpp
    • , Mark A. Newton
    • , Dennis Palagin
    • , Ana B. Pinar
    • , Marco Ranocchiari
    •  & Jeroen A. van Bokhoven
  • Article |

    Electrochemical water splitting in acidic conditions is limited by the lack of inexpensive and stable anode catalysts. Now, Simonov and colleagues report a non-noble metal-based oxygen evolution catalyst formed in situ that exhibits high stability for acidic water oxidation due to a self-healing mechanism.

    • Manjunath Chatti
    • , James L. Gardiner
    • , Maxime Fournier
    • , Bernt Johannessen
    • , Tim Williams
    • , Thomas R. Gengenbach
    • , Narendra Pai
    • , Cuong Nguyen
    • , Douglas R. MacFarlane
    • , Rosalie K. Hocking
    •  & Alexandr N. Simonov
  • Article |

    Electromicrobial production can replace fossil carbon with CO2 and electricity as feedstocks for chemical production. This work analyses and compares different electromicrobial production approaches, providing a data-driven roadmap for the sustainable and efficient implementation of this technology.

    • Nico J. Claassens
    • , Charles A. R. Cotton
    • , Dennis Kopljar
    •  & Arren Bar-Even
  • Article |

    The availability of Lewis antigens allows the investigation of their important biological functions, but site-specific fucosylation for their synthesis is challenging. This work reports an enzymatic platform for the synthesis of complex Lewis antigens, offering an opportunity to explore the Lewis antigen related glycome.

    • Jinfeng Ye
    • , Hui Xia
    • , Na Sun
    • , Chang-Cheng Liu
    • , Anran Sheng
    • , Lianli Chi
    • , Xian-Wei Liu
    • , Guofeng Gu
    • , Shu-Qi Wang
    • , Jie Zhao
    • , Ping Wang
    • , Min Xiao
    • , Fengshan Wang
    •  & Hongzhi Cao
  • Article |

    For hydrogen to become a direct, portable fuel source, the difficulties with its storage and subsequent release must be addressed. Here ethylene glycol is shown to act as an efficient, reversible liquid-to-liquid hydrogen carrier—particularly attractive due to its theoretical H2 capacity of 6.5 wt%.

    • You-Quan Zou
    • , Niklas von Wolff
    • , Aviel Anaby
    • , Yinjun Xie
    •  & David Milstein
  • Article |

    H2 is a promising mediator of electrons from electrodes to microbes for chemicals production from CO2—but its low solubility limits the productivity. This work reports nanoemulsions as H2 carriers that improve the solubility and transfer kinetics of H2, increasing the productivity of the system.

    • Roselyn M. Rodrigues
    • , Xun Guan
    • , Jesus A. Iñiguez
    • , Daniel A. Estabrook
    • , John O. Chapman
    • , Shuyuan Huang
    • , Ellen M. Sletten
    •  & Chong Liu
  • News & Views |

    The diversity of engineered amine dehydrogenases for reductive amination remains limited. Now, native amino dehydrogenases offering a different sequence space and catalytic features are discovered — enhancing and broadening the biocatalysis toolbox.

    • Andreas S. Bommarius
  • Editorial |

    Peer review has established itself as a crucial validation mechanism for modern science. Despite the disadvantages associated with its practice, it remains a powerful method to add value to scientific publications.

  • News & Views |

    Given the fact that sodium is the most abundant alkali metal on Earth, the direct and indirect use of organosodium compounds in palladium-catalysed carbon–carbon bond forming reactions is an attractive alternative for sustainable organic synthesis.

    • Henry N. C. Wong
  • News & Views |

    Good durability and activity of single Ru atom catalysts is critical for their large-scale utilization in electrochemical water splitting. Now, both of these properties can be better controlled through compressive strain engineering.

    • Boon Siang Yeo
  • News & Views |

    High-yield production of a functionally active mimic of particulate methane monooxygenase in Escherichia coli has been presented. Investigation of its catalytic mode clarifies the role of duroquinol in biomimetic methanol production.

    • Sunney I. Chan
    •  & Steve S.-F Yu
  • Article |

    Upgrading CO to high-value multicarbon products is a promising avenue for fuel and chemical feedstock production. Here triangular Cu nanosheets that selectively expose the (111) surface exhibit a high acetate partial current density (131 mA cm–2) and Faradaic efficiency (48%) in CO electroreduction.

    • Wesley Luc
    • , Xianbiao Fu
    • , Jianjian Shi
    • , Jing-Jing Lv
    • , Matthew Jouny
    • , Byung Hee Ko
    • , Yaobin Xu
    • , Qing Tu
    • , Xiaobing Hu
    • , Jinsong Wu
    • , Qin Yue
    • , Yuanyue Liu
    • , Feng Jiao
    •  & Yijin Kang
  • Perspective |

    CO2 hydrogenation is frequently acclaimed as a strategy for greenhouse gases mitigation, although the carbon footprint of the corresponding electrocatalytic or thermocatalytic process is often neglected. This Perspective analyses the amount of CO2 generated during methanol production for different catalytic processes and hybrid thereof.

    • Brian M. Tackett
    • , Elaine Gomez
    •  & Jingguang G. Chen
  • Article |

    Immobilized molecular catalysts can be efficient for the electroreduction of CO2, but their practical applicability is hampered by the continued use of rare metals. Here, a photoelectrode based on an earth-abundant molecular catalyst with high CO2 reduction performance is introduced.

    • Jane J. Leung
    • , Julien Warnan
    • , Khoa H. Ly
    • , Nina Heidary
    • , Dong Heon Nam
    • , Moritz F. Kuehnel
    •  & Erwin Reisner
  • Article |

    In heterogeneous catalysis, solvents—and their interaction with metal supports—have a complex effect on reactivity. This study shows that, in Pd-catalysed furfural hydrogenation, water influences the rate and selectivity by favouring a proton transfer rather than a purely surface-bound mechanism.

    • Zheng Zhao
    • , Reda Bababrik
    • , Wenhua Xue
    • , Yaping Li
    • , Nicholas M. Briggs
    • , Dieu-Thy Nguyen
    • , Umi Nguyen
    • , Steven P. Crossley
    • , Sanwu Wang
    • , Bin Wang
    •  & Daniel E. Resasco
  • Article |

    Methane monooxygenase (MMO)—a protein of high biotechnological interest for the selective and mild conversion of methane to methanol—lacks a high-throughput production system. Now, the authors report the efficient production of particulate MMO-mimics for catalysis in solution and hydrogels.

    • Hyun Jin Kim
    • , June Huh
    • , Young Wan Kwon
    • , Donghyun Park
    • , Yeonhwa Yu
    • , Young Eun Jang
    • , Bo-Ram Lee
    • , Eunji Jo
    • , Eun Jung Lee
    • , Yunseok Heo
    • , Weontae Lee
    •  & Jeewon Lee
  • Article |

    Axially chiral biaryls have proven to have a wide variety of uses—perhaps most importantly as ligands in asymmetric catalysis—but their synthesis remains challenging. Here, Bin Tan and colleagues report a redox-neutral aryl–aryl coupling, providing a direct route to N,N and N,O axially chiral biaryls in high yields and enantioselectivities.

    • Liang-Wen Qi
    • , Shaoyu Li
    • , Shao-Hua Xiang
    • , Jun (Joelle) Wang
    •  & Bin Tan
  • Article |

    A common problem with double C–H activation/cross-coupling is the formation of homocoupled products. Here, the authors show that an ionic group on one reagent during Fe catalysed cross-couplings can lead to a clearly defined order of C–H activation and hence the avoidance of homocoupled side-products.

    • Takahiro Doba
    • , Tatsuaki Matsubara
    • , Laurean Ilies
    • , Rui Shang
    •  & Eiichi Nakamura
  • Article |

    New enzymes for the efficient and stereoselective synthesis of chiral amines are of high interest for the pharmaceutical industry. Now, Grogan, Vergne-Vaxelaire and co-workers report the discovery, characterization, crystal structure and engineering of a family of native amine dehydrogenases for the preparation of chiral amines from ketones.

    • Ombeline Mayol
    • , Karine Bastard
    • , Lilian Beloti
    • , Amina Frese
    • , Johan P. Turkenburg
    • , Jean-Louis Petit
    • , Aline Mariage
    • , Adrien Debard
    • , Virginie Pellouin
    • , Alain Perret
    • , Véronique de Berardinis
    • , Anne Zaparucha
    • , Gideon Grogan
    •  & Carine Vergne-Vaxelaire
  • Perspective |

    The electrochemical reduction of nitrogen is being intensely investigated as the basis for future ammonia production. This Perspective critiques current steps and missteps towards this goal in terms of experimental methodology and catalyst selection, proposing a protocol for rigorous experimentation.

    • Bryan H. R. Suryanto
    • , Hoang-Long Du
    • , Dabin Wang
    • , Jun Chen
    • , Alexandr N. Simonov
    •  & Douglas R. MacFarlane
  • Article |

    While organolithium and organomagnesium compounds have well developed methods in organic chemistry, organosodium compounds are much less widely used. Here a method to generate organosodium compounds from aryl chlorides and (hetero)arenes is reported, along with a demonstration of their use in cross-coupling reactions.

    • Sobi Asako
    • , Hirotaka Nakajima
    •  & Kazuhiko Takai
  • News & Views |

    The synthesis of highly branched low molecular weight products — potential synthetic lubricants — directly from ethylene is challenging when highly efficient early transition metal catalysts are employed. Now, an alkane soluble co-catalyst permits the synthesis of such polyethylenes using a zirconium catalyst in a saturated hydrocarbon solvent, where competitive solvent coordination at the active site of the catalyst is relatively unimportant.

    • Rhett Kempe
  • News & Views |

    The asymmetric synthesis of chiral γ-lactams is difficult and laborious; typically requiring pre-functionalization of starting materials. Now, a highly efficient alternative approach employing direct C−H amidation via chiral hydrogen-bond-donor catalysts has been developed.

    • Tong-De Tan
    •  & Long-Wu Ye
  • News & Views |

    The selective electrochemical conversion of ketones to value-added products still represents a challenge, due to a lack of fundamental understanding. Now, a principle has been revealed that allows the steering of the electroreduction of aliphatic ketones on platinum by carefully controlling the coordination number of the platinum atoms.

    • Ivana Matanović
  • Review Article |

    Photocatalytic water splitting with particulate semiconductors represents a promising strategy for the generation of hydrogen as a solar fuel. This review covers recent advances in the development of reaction systems and photocatalysts towards the scale-up of this technology, emphasizing at the same time the challenges to overcome.

    • Takashi Hisatomi
    •  & Kazunari Domen
  • Article |

    While Ru-based electrocatalysts are among the most active for acidic water oxidation, they suffer from severe deactivation. Now, Yuen Wu, Wei-Xue Li and co-workers report a core–shell Ru1–Pt3Cu catalyst with surface-dispersed Ru atoms for a highly active and stable oxygen evolution reaction in acid electrolyte.

    • Yancai Yao
    • , Sulei Hu
    • , Wenxing Chen
    • , Zheng-Qing Huang
    • , Weichen Wei
    • , Tao Yao
    • , Ruirui Liu
    • , Ketao Zang
    • , Xiaoqian Wang
    • , Geng Wu
    • , Wenjuan Yuan
    • , Tongwei Yuan
    • , Baiquan Zhu
    • , Wei Liu
    • , Zhijun Li
    • , Dongsheng He
    • , Zhenggang Xue
    • , Yu Wang
    • , Xusheng Zheng
    • , Juncai Dong
    • , Chun-Ran Chang
    • , Yanxia Chen
    • , Xun Hong
    • , Jun Luo
    • , Shiqiang Wei
    • , Wei-Xue Li
    • , Peter Strasser
    • , Yuen Wu
    •  & Yadong Li
  • Perspective |

    The hydrogenation of CO2 to form methane has been known for over a century. However, given increased interest in small-molecule activation for energy storage, and improved catalysts and understanding of the process, it is worthwhile to look again at the reaction. This Perspective discusses recent work on the fundamentals of the Sabatier reaction and also the potential for large-scale applications.

    • Charlotte Vogt
    • , Matteo Monai
    • , Gert Jan Kramer
    •  & Bert M. Weckhuysen
  • Review Article |

    The electrochemical reduction of carbon dioxide to fuels and feedstocks has received increased attention over the past few years. In this Review, Roldan Cuenya and co-workers discuss strategies to achieve high selectivity towards multicarbon products via rational catalyst and electrolyte design.

    • Dunfeng Gao
    • , Rosa M. Arán-Ais
    • , Hyo Sang Jeon
    •  & Beatriz Roldan Cuenya
  • Article |

    The electrocatalytic reduction of carbonyl groups is gaining attention in the context of biorefinery. However, fundamental knowledge on such processes is still limited. Now, the selectivity for the electroreduction of acetone on platinum single crystals is studied, revealing a remarkable structural sensitivity.

    • Christoph J. Bondue
    • , Federico Calle-Vallejo
    • , Marta C. Figueiredo
    •  & Marc T. M. Koper
  • Article |

    The electrochemical reduction of nitrogen to ammonia represents a challenge of major interest that would substantially decrease the burden of the energy-consuming Haber–Bosch process. Now, Yin, Yan, Zhang, Si and colleagues achieve high ammonia yield and Faradaic efficiency over 66% using bismuth nanocatalysts promoted by alkali cations.

    • Yu-Chen Hao
    • , Yu Guo
    • , Li-Wei Chen
    • , Miao Shu
    • , Xin-Yu Wang
    • , Tong-An Bu
    • , Wen-Yan Gao
    • , Nan Zhang
    • , Xin Su
    • , Xiao Feng
    • , Jun-Wen Zhou
    • , Bo Wang
    • , Chang-Wen Hu
    • , An-Xiang Yin
    • , Rui Si
    • , Ya-Wen Zhang
    •  & Chun-Hua Yan
  • Article |

    Iron single-atom catalysts are among the most promising fuel cell cathode materials in acid electrolyte solution. Now, Shui, Xu and co-workers report concave-shaped Fe–N–C nanoparticles with increased availability of active sites and improved mass transport, meeting the US Department of Energy 2018 target for platinum-group metal-free fuel cell catalysts.

    • Xin Wan
    • , Xiaofang Liu
    • , Yongcheng Li
    • , Ronghai Yu
    • , Lirong Zheng
    • , Wensheng Yan
    • , Hui Wang
    • , Ming Xu
    •  & Jianglan Shui
  • Article |

    Metal oxides have been identified as a promising class of catalysts for carbon–oxygen bond cleavage in the context of biomass valorization, although the systematic understanding of their reactivity remains elusive. Now, a combination of catalytic screening and first principles calculations provide important insights into this family of catalysts.

    • Konstantinos A. Goulas
    • , Alexander V. Mironenko
    • , Glen R. Jenness
    • , Tobias Mazal
    •  & Dionisios G. Vlachos
  • Article |

    Low-molecular-weight, highly branched polyethylenes are attractive candidates for synthetic lubricants, but their efficient production is constrained by a lack of effective catalytic methods. While conventional group IV transition metal catalysts produce diverse polyethylenes on a huge scale, they are unable to produce highly branched polyethylenes. Here a hydrocarbon-soluble organozirconium precatalyst and borate cocatalyst produce the desired polyethylenes with excellent activity and branch selectivity.

    • Yanshan Gao
    • , Jiazhen Chen
    • , Yang Wang
    • , David B. Pickens
    • , Alessandro Motta
    • , Q. Jane Wang
    • , Yip-Wah Chung
    • , Tracy L. Lohr
    •  & Tobin J. Marks
  • Article |

    Copper on ceria is an excellent catalyst for the low-temperature water–gas shift reaction. Here the active sites are directly imaged by electron microscopy and probed with in situ spectroscopy, showing that the reaction proceeds via a cooperative mechanism whereby the Cu+ chemically adsorbs CO while an adjacent Ov–Ce3+ site dissociatively activates H2O.

    • Aling Chen
    • , Xiaojuan Yu
    • , Yan Zhou
    • , Shu Miao
    • , Yong Li
    • , Sebastian Kuld
    • , Jens Sehested
    • , Jingyue Liu
    • , Toshihiro Aoki
    • , Song Hong
    • , Matteo Farnesi Camellone
    • , Stefano Fabris
    • , Jing Ning
    • , Chuanchuan Jin
    • , Chengwu Yang
    • , Alexei Nefedov
    • , Christof Wöll
    • , Yuemin Wang
    •  & Wenjie Shen
  • Article |

    Photoelectrochemical cells have been widely used for the production of solar fuels, but have seen limited applications in organic synthesis. Here the authors demonstrate photoelectrocatalytic C–H amination of aromatics, using haematite as the photoanode.

    • Lei Zhang
    • , Laurent Liardet
    • , Jingshan Luo
    • , Dan Ren
    • , Michael Grätzel
    •  & Xile Hu
  • Article |

    Chiral γ-lactams are of significant interest being present in numerous pharmaceutical agents; however, their chemical synthesis is complex, requiring pre-functionalized starting materials. Now, Park and Chang report an iridium-based catalyst system for the production of chiral γ-lactams from an abundant feedstock via an intramolecular asymmetric sp3 C−H amidation.

    • Yoonsu Park
    •  & Sukbok Chang