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This is the 28th volume of Memorial Tributes compiled by the National Academy of Engineering as a personal remembrance of the lives and outstanding achievements of its members and international members. These volumes are intended to stand as an enduring record of the many contributions of engineers and engineering to the benefit of humankind. In most cases, the authors of the tributes are contemporaries or colleagues who had personal knowledge of the interests and the engineering accomplishments of the deceased. Through its members and international members, the Academy...
This is the 28th volume of Memorial Tributes compiled by the National Academy of Engineering as a personal remembrance of the lives and outstanding achievements of its members and international members. These volumes are intended to stand as an enduring record of the many contributions of engineers and engineering to the benefit of humankind. In most cases, the authors of the tributes are contemporaries or colleagues who had personal knowledge of the interests and the engineering accomplishments of the deceased. Through its members and international members, the Academy carries out the responsibilities for which it was established in 1964.
Under the charter of the National Academy of Sciences, the National Academy of Engineering was formed as a parallel organization of outstanding engineers. Members are elected on the basis of significant contributions to engineering theory and practice and to the literature of engineering or on the basis of demonstrated unusual accomplishments in the pioneering of new and developing fields of technology. The National Academies share a responsibility to advise the federal government on matters of science and technology. The expertise and credibility that the National Academy of Engineering brings to that task stem directly from the abilities, interests, and achievements of our members and international members, our colleagues and friends, whose special gifts we remember in this book.
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BY ARUMUGAM MANTHIRAM AND M. STANLEY WHITTINGHAM
JOHN BANNISTER GOODENOUGH, a world-renowned materials scientist and Nobel laureate in chemistry, died on June 25, 2023, at the age of 100. He was born to American parents, Erwin Ramsdell and Helen Miriam (Lewis) Goodenough, in Jena, Germany, on July 25, 1922. His parents were enjoying a long summer vacation in Germany while his father was completing a DPhil dissertation at the University of Oxford. John was the second of six children. In 1925, the family returned to their home in Woodbridge, Connecticut, just seven miles north of Yale University. His father later worked as an assistant professor in Yale’s Department of History.
As a young man, Goodenough attended the Foote School in New Haven, Connecticut. In 1934, he was admitted to the Groton School, from which he graduated magna cum laude in 1940 with the top grade in his class. He entered Yale University in 1940 and graduated in 1944 with a bachelor’s degree in mathematics, summa cum laude. At Yale, he was a member of Skull and Bones, a secret society of senior students. More details about his early education can be found in his book Witness to Grace (Publish America, 2008).
During World War II, with one year of study left to complete at Yale, Goodenough enlisted in the U.S. Army Air Corps in 1942 and joined the Army in 1943. He was stationed as a meteorologist at an air base in Houlton, Maine, a few miles south of Presque Isle, the northeastern-most town in the United States, to dispatch fighter planes to England. He had the solemn responsibility of forecasting not only wind patterns and speeds at flight level across the Atlantic, but also the weather en route and at the final destination. After the war ended in 1945, he was selected as one of 21 returning officers chosen to pursue graduate study in physics or mathematics at either the University of Chicago or Northwestern University.
While still holding the rank of captain under the Quartermaster Corps, in 1946 Goodenough chose to pursue graduate studies in physics at the University of Chicago. When he went to register, one of his professors told him, “I don’t understand you veterans. Don’t you know that anyone who has ever done anything significant in physics had already done it by the time he was your age; and you want to begin?”1 He opted to conduct his research in solid-state physics, with Professor Clarence Zener (NAS) as his supervisor. When he arrived at Zener’s office, Zener told him, “Yes, you can be my student. Now you have two things you must do. The first thing is to find your research problem and the second thing is to solve it. Good Day!”2 Goodenough chose the calculation of the interaction of the Fermi surface with the Brillouin zone boundaries of noncubic metal alloys as his Ph.D. dissertation topic. When Zener left to become the director of the Westinghouse Research Laboratory in Pittsburgh, Goodenough had the opportunity, during his final year of graduate studies, to work as a research engineer at Westinghouse. He received his M.S. degree in 1951 and Ph.D. in 1952, both in physics. In 1951, he married Irene Wiseman.
In 1952, Goodenough joined the Lincoln Laboratory at the Massachusetts Institute of Technology (MIT) as a research engineer. At that time, digital computers ran on large vacuum tubes and had no memory. Goodenough was assigned to a small group responsible for developing insulating magnetic materials with a square M-H hysteresis loop, where M refers to magnetization and H refers to applied magnetic field. The goal was to build random access memory (RAM) with a fast read-rewrite switching time. As a physicist, he recognized the importance of working with skilled solid-state chemists who could effectively synthesize and characterize materials. He also understood the value of interdisciplinary collaboration and how bridging the gap between chemistry and physics could drive engineering innovations. Using a systematic empirical approach and introducing quality control, his team optimized the firing/annealing time, temperature, and cooling rate for iron-based spinel oxides. This allowed them to fabricate polycrystalline ceramic cores with the required square M-H hysteresis loop. Goodenough’s key contribution was identifying the factors that control the shape of the M-H loop.
During this work, Goodenough was able to recognize the following two-part fundamental understanding: (i) the atomic order occurring in those spinel oxides at the annealing temperature is related to a critical concentration of manganese in the material; and (ii) the occurrence of a cubic-to-tetragonal structural transition above the critical manganese concentration is due to a cooperative orbital ordering in manganese. This insight was fundamental in determining crystal structure symmetry. It is now known as the Jahn-Teller distortion effect, named after Hermann Jahn and his student Edward Teller (NAS), who previously demonstrated that a molecule in high symmetry with orbital degeneracy will distort to lower symmetry by removing the degeneracy and becoming more stable.
By investigating the magnetic properties of various oxides, Goodenough formulated the rules for magnetic interactions in solids based on crystal structure and chemical bonding. The rules predict ferromagnetic versus antiferromagnetic interactions based on electronic configuration, bond angle, metal-metal interactions versus metal-nonmetal interactions, and other factors. These are now known as the Goodenough-Kanamori rules, as Junjiro Kanamori later provided the mathematical formalism that justifies them. A detailed explanation of these rules can be found in Magnetism and the Chemical Bond (Interscience, 1963), Goodenough’s textbook.
When his Lincoln Lab group successfully demonstrated the first magnetic memory for digital computers, they were all called into Goodenough’s boss’s office on a Friday afternoon. After a one-minute thank you for their work, his boss asked, “And now that you have worked yourselves out of a job, what are you planning to do?”3 Half of the group chose to take their expertise to industry. After considering his options for a few days, Goodenough decided to work on magnetic-film memory, aiming to switch all individual atomic magnetic moments simultaneously instead of sequentially. Unfortunately, attempts to achieve reliable film switching resulted in slower switching times. Therefore, he turned to focusing on investigating how competing interactions between atomic magnetic moments could lead to unexpected, complex magnetic order — as well as how the role of cooperative orbital ordering could lead to magnetostrictive phenomena that could be used in devices. These concepts are also presented in his book, Magnetism and the Chemical Bond.
While at Lincoln Lab, Goodenough also systematically pursued the transition from localized to itinerant electron behavior by working with transition-metal oxides and sulfides. He recognized that intraatomic interactions localize the electrons to an atomic site, while interatomic interactions between atoms delocalize the electrons and belong equally to all like atoms in a periodic array. As a result of this recognition, he explained and predicted metal-insulator transitions in oxides, such as in vanadium dioxide with the rutile structure, and the associated crystal symmetry and phase transformations. His fundamental understanding at the crossover between the localized electron regime to itinerant electron regime in solids led him to publish a 1971 review article entitled “Metallic Oxides.”4
Around 1970, an amendment to a bill passed by the U.S. Congress prohibited research in laboratories like Lincoln Lab not targeted towards specific governmental applications. Therefore, Goodenough was ordered to terminate his fundamental research. This turned his attention towards renewable energy and energy conversion, particularly the electrolysis of water to produce hydrogen but the use of exhaust heat from power plants in a solid oxide fuel cell. During his time at Lincoln Lab, he developed the sodium superionic conductor (NASICON) with a framework structure, which in recent years has become a potential structure for solid-state electrolytes. However, he was informed that Lincoln Lab, as an Air Force lab, could not pursue energy-related research, which was designed for national energy laboratories and industry.
In the meantime, Goodenough was thinking about the best ways to bring technologies to the developing world. In 1974, he was invited to head up a research lab focused on energy in Tehran, Iran. While he was seriously considering the offer, he received a letter from the University of Oxford requesting him to apply for the head position at the Inorganic Chemistry Laboratory. Traditionally, the Inorganic Chemistry Lab had been headed up by a solid-state chemist, but the position interested Goodenough since it would also give him an opportunity as a physicist to collaborate with chemists. With encouragement from his wife — even though she would be giving up her teaching job at a community college in Massachusetts — Goodenough declined the offer from Iran and joined Oxford in 1976.
Although transitioning from a U.S. government research lab to head up a department at Oxford might have seemed challenging, Goodenough experienced a smooth transition, as most teaching and coaching was handled by instructors. As a professor at Oxford, he had full freedom to choose his research focus, unlike in a U.S. national lab. To fulfill his desire to help society, he chose to work on energy-related problems, beginning with direct methanol fuel cells and the photoelectrolysis of water. However, he faced the challenge of finding an electrocatalyst with sufficient electrocatalytic activity below 100°C for methanol oxidation at the anode (negative electrode) in a fuel cell. This challenge, along with his interest on photoelectrolysis, involved him in electrochemistry at Oxford.
Around the time he left Lincoln Lab, he became aware of M. Stanley Whittingham’s (NAE 2018) illustration of a rechargeable lithium battery at what was then Exxon Corporation in the United States.5 Whittingham used a lithium-metal anode (negative electrode) and titanium sulfide (TiS2) cathode (positive electrode). TiS2 had a layered structure, in which edge-shared TiS6 octahedral sheets were held together by Van der Waals forces. Upon discharging the cell (inserting lithium ions into the Van der Walls gap between the TiS2 sheets), the direct metal-metal (Ti-Ti) interactions along the shared edges in LixTiS2 (0 ≤ x ≤ 1) solid solution provided metallic conductivity, a desired feature for functioning as an electrode in an electrochemical device. The Li-TiS2 cell offered a cell voltage of less than 2.4V.
Whittingham’s work spurred immense interest and activity in the chemistry community, leading researchers to investigate various transition-metal chalcogenides (sulfides and selenides) with layered structures. While this scientific endeavor was taking place, some battery companies began assembling cells and introducing them to the market.
Unfortunately, the use of lithium metal as an anode posed safety concerns, as it led to the formation of lithium dendrites, which could cause short-circuiting and fire hazards. As a result, in the 1980s, companies were forced to abandon the commercialization and marketing of rechargeable lithium batteries.
While getting involved with electrochemistry at Oxford, Goodenough recognized, based on his nearly three decades of work on the physics and chemistry of solids, that it would not be possible to achieve a voltage greater than 2.5V with a sulfide or selenide cathode. Because the top of the S2-:3p and Se2-:4p bands lie high in energy, it would be difficult to access higher oxidation states of transition metals and lower the cathode redox energy. This limitation would prevent the increase of cell voltage beyond 2.5V. As a result, pairing a lithium insertion-compound anode with a sulfide or selenide cathode would not generate sufficient cell voltage to be practical and competitive with aqueous rechargeable batteries.
This recognition led Goodenough to consider transition-metal oxides as cathodes because the top of the O2-:2p band lies at a lower energy than S2-:3p or Se2-:4p bands. However, while MO2 (M = transition metal) oxides were analogous to layered TiS2, it was unclear whether their M3+/4+ redox energy was low enough to maximize the cell voltage, and they could not be synthesized. Therefore, Goodenough turned his attention to layered transition-metal oxides that already contained lithium while at the same time possessing low enough M3+/4+ redox energies. This inspired him and his research group of experimental chemists at Oxford — including a visiting experimental physicist, Shuichi Mizushima, from the University of Tokyo — to explore LiMO2 oxides with M = Cr, Co, and Ni. In 1980, they found that a significant amount of lithium could be extracted with M = Co or Ni, while still maintaining the layered structure at an operating cell voltage of 4V.
Following the identification of layered LiMO2 oxides as cathodes, Michael Thackeray (NAE 2021) arrived at Oxford from South Africa to work with Goodenough as a visiting chemist. Prior to his arrival, Thackeray had been investigating lithium insertion into Fe3O4 spinel, an oxide much cheaper than LiCoO2, with the aim being to reduce cost. However, Goodenough was skeptical of lithium insertion into the spinel structure because he thought the spinel structure could not accommodate additional cations like lithium in them. While working together at Oxford, Goodenough asked Thackeray to investigate lithium insertion into LiMn2O4 spinel. They found that lithium could indeed be inserted into LiMn2O4 spinel, forming Li2Mn2O4 (0 ≤ x ≤ 1) spinel at 3V — but they discovered all the lithium ions existing in the tetrahedral sites were displaced to the neighboring octahedral sites along with the inserted lithium ions to reduce electrostatic repulsion. However, it operated at a lower voltage of 3V with a flat voltage profile due to the existence of a two-phase region consisting of the cubic spinel phase Li2Mn2O4 and an ordered rock-salt phase Li2Mn2O4 with tetragonal symmetry due to the cooperative Jahn-Teller distortion associated with Mn3+, which contained a single electron in the eg band. Despite this distortion, the ordered rock-salt Li2Mn2O4 maintained the three-dimensional M2O4 spinel framework.
The large instantaneous change in the c/a ratio during the cubic-to-tetragonal phase transition made the reversible insertion and extraction of lithium over many cycles challenging, resulting in capacity fade during charge-discharge. However, they showed that lithium could be extracted reversibly from cubic LiMn2O4 spinel to give cation-deficient cubic spinel Mn2O4 (referred to as l-MnO2) at 4V. The extraction and insertion of lithium from and into the tetrahedral sites in Li1-xMn2O4 (0 ≤ x ≤ 1) instead of the octahedral sites in Li1+xMn2O4 (0 ≤ x ≤ 1) resulted in a 1V increase. This finding led them to recognize the importance of the lithium-site energy contribution to the redox energy of transition-metal ions.
In November 1985, Arumugam Manthiram arrived at Oxford from India to work with Goodenough as a visiting chemist; by then, both Mizushima and Thackeray had returned to their home countries to resume their previous jobs. Based on Manthiram’s Ph.D. dissertation work in India with the polyanion oxides Ln2(MoO4)3 (Ln = lanthanide) as a means to further reduce cathode cost beyond cobalt and manganese, he and Goodenough explored lithium insertion into Fe2(MoO4)3. They found two lithium ions per molecule could be inserted and extracted reversibly with a flat voltage of 3V, due to the formation of a two-phase region consisting of Fe2(MoO4)3 and Li2Fe2(MoO4)3.
In September 1986, Goodenough, at the age of 64, accepted an endowed chair position and joined the University of Texas at Austin (UT Austin). His decision to move — after 10 years at Oxford — was influenced by England’s mandatory retirement policy at age 65, and his desire to return to his home country. After a 10-month stay with Goodenough at Oxford, Manthiram accompanied him to UT Austin and was tasked with setting up their solid-state chemistry lab. As Goodenough and Manthiram settled into their new roles, the observation of superconductivity with a high-transition temperature in copper oxides became a hot topic in the physics and chemistry communities. Along with Jianshi Zhou, a visiting student from China, they worked on the synthesis, characterization, and physical measurements of copper oxide superconducting materials.
While engaged with copper oxide superconductors, Manthiram and Goodenough continued to explore other iron-based polyanion oxides like Fe2(SO4)3 with the same structure as Fe2(MoO4)3 in order to reduce the weight of the cathode since sulfur is much lighter than molybdenum. In 1989, they found that Fe2(SO4)3 delivered a flat voltage of 3.6V, compared to 3.0V for both Fe2(MoO4)3 and Fe2(WO4)3, despite having the same Fe2+/3+ redox couple and identical structure. This led to them recognizing the role of the ionicity of the X-O bond in the polyanion XO4 (X = Mo, W, and S) in altering the covalency of the Fe-O bond through the inductive effect and its impact on redox energy. The higher covalent character of the S-O bond compared to the Mo-O or W-O bond decreased the covalency of the Fe-O bond through inductive effect and thereby lowered the Fe2+/3+ redox energy and increased the cell voltage.
In the 1990s, intrigued by these findings, Goodenough focused on investigating a number of polyanion oxides alongside his graduate student, Padhi, and postdoc Nanjundaswamy. In 1997, their efforts led to the identification of LiFePO4, along with other LiMPO4 (M = Mn, Co, and Ni) compounds with the olivine structure, as potential cathodes.6 While LiFePO4 operates with a flat voltage at 3.4V, LiMnO4 operates at approximately 4V, and LiCoO4 even at a higher voltage of 4.8V. The polyanion oxides, including the initial M2(XO4)3 structure initially studied by Manthiram and Goodenough, have now become a broad family of electrodes for lithium-ion and sodium-ion batteries.
At UT Austin, Goodenough spent the next 37 years researching electrode and solid-state electrolyte materials for lithium-based and sodium-based batteries. Later, he became heavily engaged with all-solid-state batteries with the aim being to enhance battery safety since liquid electrolytes are prone to fire hazard. In addition, he focused on the design and development of both oxide-ion conducting solid electrolytes and using electrocatalysts for solid oxide fuel cells.
While keeping himself engaged with battery and fuel cell materials, he never lost sight of his core interest in the physics of transition-metal oxides. His heart was always very much with the localized versus itinerant behavior of oxides, orbital ordering, and lattice instabilities that could occur at the transition from localized to itinerant electron regime — as well as the unusual physical phenomena these transitions could produce. Examples include the discovery of high-temperature superconductivity in copper oxides and colossal magnetoresistance in manganese oxides.
Seven decades of Goodenough’s contributions to science and engineering at three marvelous institutions — Lincoln Lab, Oxford, and UT Austin — bridged the gap between chemistry and physics with an eye towards targeted engineering technologies, all of which had a profound impact on humanity. The development of random access memory for digital computers and the use of oxide cathodes for lithium-ion batteries are two examples of his engineering breakthroughs. Inspired by Whittingham’s illustration of rechargeable lithium batteries with intercalation electrodes, Goodenough developed oxide cathodes with higher operating voltages, eliminating the need for a lithium-metal anode. His cathode, combined with a carbonaceous anode by Akira Yoshino, led to the lithium-ion technology that has become an integral part of our daily life. This groundbreaking achievement was the basis for the 2019 Nobel Prize in Chemistry awarded to Whittingham, Goodenough, and Yoshino. Goodenough was able to accomplish these engineering and fundamental science breakthroughs by focusing uniquely at the interface between chemistry and physics, collaborating with experts in complementary fields. His commitment to interdisciplinarity and his ability to work closely with chemists at all three institutions was his trademark.
In addition to the Nobel Prize, his contributions have led to his receiving numerous prestigious awards and honors over the years — including the National Medal of Science for Engineering (2013), the Copley Medal of the Royal Society (2019), the Fermi Award (2019), the Japan Prize (2001), the Draper Prize (2014), and the Von Hippel Award (1989), just to name a few. During his 100th birthday celebration in July 2022, the Electrochemical Society established the John B. Goodenough Award in his honor to commemorate his invaluable contributions to the scientific community. The award recognizes outstanding contributions to materials innovations in batteries, solid ion conductors, fuel cells, transition-metal oxides, and magnetic materials — encompassing the broad areas in which he was profoundly engaged.
Goodenough’s contributions were not confined to the boundaries of his research laboratory or the fields of science and engineering. He was a man of profound faith and love. Inspired by Endicott Peabody during his formative years at Groton School, he embraced the fundamentals of Christianity and compassion for his fellow human beings. His math professor at Yale, Egbert Miles, played a pivotal role in enriching and shaping his academic journey. Goodenough was fond of using poetry as a medium of expression, which allowed him to overcome dyslexia and convey his love and affection for his beloved wife, Irene.
Beyond his contributions to humanity, Goodenough is distinguished by his unique personal characteristics. He displayed a unique and memorable blending of intellect and modesty with love and respect for everyone. One seldom sees such a combination. He was known for his humility, kindness, and willingness to mentor and collaborate with fellow scientists and students — while at the same time, even at an advanced age, being eager to learn from others. His distinct laugh while conversing is unforgettable! Led by his faith, he always combined a sense of purpose with unwavering moral integrity. Goodenough and his wife Irene shared a spirit of love, a commitment to knowledge, and a relentless pursuit of scientific excellence. He remains a role model and an inspiration to all.
Goodenough described his remarkable journey, in 2008, in his book, Witness to Grace. The book shares his life story, professional journey, and Christian pilgrimage. Serving as a testament to his character, it reveals the depth of his dedication to both scientific inquiry and spiritual growth. As a fitting tribute to his lifelong pursuit of knowledge and wisdom, he presented a copy of this book to the Nobel Prize Library in 2019.
Irene Wiseman died in 2016. Goodenough and his wife had no children. He is survived by his half sister, Ursula W. Goodenough, and his half brother, Daniel A. Goodenough.
____________________________________ 1 Goodenough JB. 2008. Witness to Grace. Publish America. 2 Goodenough JB. 2008. Witness to Grace. Publish America. 3 Goodenough JB. 2008. Witness to Grace. Publish America. 4 Goodenough JB. 1971. Metallic oxides. Progress in Solid State Chemistry 5:145-399. 5 Whittingham MS. 1976. Electrical energy storage and intercalation chemistry. Science 192(4244):1126-27. 6 Padhi AK, Nanjundaswamy KS, Goodenough JB. 1997. Phospho-olivines as positive electrode materials for rechargeable lithium batteries. Journal of the Electrochemical Society 144(4):1188-94.